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This study explores the contribution of glass phase and rubber phase to polymer failure, and establishes a theoretical model of temperature‐dependent tensile strength (TDTS) considering the effect of two‐phase transition based on the Force‐heat Equivalence Energy Density Principle (FHEEDP). The model achieves good verification by comparison with the TDTS experimental data of various polymer materials, including epoxy‐based shape memory polymer (SMP), PEEK‐based SMP and CdS/PMMA. The results demonstrate that the model can perform an accurate prediction for the tensile strength of polymer at different temperatures by easily obtainable material parameters. In conclusion, the proposed theoretical model deepens the understanding on the two‐phase transition and their effect on the TDTS, as well as supplies a practical predicted method on the TDTS of polymer, which is crucial for polymer applied in extreme condition. [ABSTRACT FROM AUTHOR]

The performance of machine learning algorithms is conditioned by the availability of training datasets, which is especially true for the field of nondestructive evaluation. Here we propose one reconfigurable specimen instead of numerous reference specimens with known, unchangeable defect properties, which are usually complicated to fabricate. It consist of a shape memory polymer foil with temperature-dependent Young's modulus and ultrasound attenuation. This open a possibility to generate a reconfigurable defect by projecting a heating laser in the form of a short line on the specimen surface. Ultrasound is generated by a laser pulse at one fixed position and detected by a laser vibrometer at another fixed position for 64 different defect positions and 3 different configurations of the specimen. The obtained diversified datasets are used to optimize the neural network architecture for the interpretation of ultrasound signals. We study the performance of the model in cases of reduced and dissimilar training datasets. In our first study, we classify the specimen configurations with the defect position being the disturbing parameter. The model shows high performance on a dataset of signals obtained at all the defect positions, even if trained on a completely different dataset containing signals obtained at only few defect positions. In our second study, we perform precise defect localization. The model becomes robust to the changes in the specimen configuration when a reduced dataset, containing signals obtained at two different specimen configurations, is used for the training process. This work highlights the potential of the demonstrated machine learning algorithm for industrial quality control. High-volume products (simulated by a reconfigurable specimen in our work) can be rapidly tested on the production line using this single-point and contact-free laser ultrasonic method. [ABSTRACT FROM AUTHOR]

To construct resilient structures, systems and sustainable buildings, capable of enduring fatigue, inclement weather, and seismic activity, researchers are actively seeking effective solutions to minimize vibrations and cyclic loading. Although these factors may not have immediate effects, they contribute to residual deformation in structures that gradually grows over time. For this reason, shape memory alloy (SMA) can be used as a perfect damper to dissipate the mechanical load in structures construction and buildings. The SMA actuators characterized by several thermo-mechanical functions, they are generally used in different applications as Mechatronics, Biomedical, Mechanical engineering and building systems. This study aims to adapt SMA actuator with structures for construction and buildings, in order to ensure a high displacement and vigilance taking into account fatigue phenomena to repulse mechanical fatigue and fretting. Accordingly, a thermomechanical analysis has been developed using finite element techniques to describe shape memory alloys' behavior and can integrate these material as a thermomechanical actuator dampers in building engineering systems. Furthermore, the suggested model elucidates the actuator's thermomechanical response, showcasing its adaptable behavior to both superelasticity and the shape memory effect within the desired structure in the building. Thus, the numerical findings affirm the efficacy of the proposed design that based on shape memory materials in addressing thermomechanical fatigue within buildings, concurrently enhancing structural resilience against mechanical fatigue. The primary outcome of this study is the successful preservation of the Ni-Ti superelastic response within the proposed system. This preservation is validated through cycling variations of up to 7.6% strain, significantly surpassing the requirements typically mandated for applications in earthquake engineering. [ABSTRACT FROM AUTHOR]

Highlights Fabric‐reinforced shape memory polymeric composites (SMPC) have shown great potential in the design of intelligent deformation structures. In this work, the weft‐knitted fabric inserted with weft yarns was developed as reinforcement to fabricate the shape memory epoxy polymer (SMEP) composites. The effects of weft yarn, loop density and direction on the shape memory performance of SMPC under different bending radii were experimentally investigated. The results show that the SMPC have good shape fixity ratios and shape recovery ratios of around 98%. As compared with those of SMPCs without inserting weft yarns, the SMPCs with weft yarns have shorter shape recovery time, and the recovery force of SMPCs with weft yarns in the 0° and 90° directions shows an increase of 86.4% and 79.5%, respectively. The recovery force of SMPC improve 3.7 times compared to SMEP. The multiscale models of SMPC were established with basis of the results of micro‐computed tomography scanning of specimens and viscoelastic theory. The surface buckling behaviors of SMEP and SMPC specimens after U‐bending load were discussed. Finally, the deformation of loops and weft yarns of SMPC were analyzed to reveal the shape memory mechanism. Shape memory polymeric composites (SMPC) with weft yarns has shorter shape recovery time. Recovery force of SMPC with weft yarns was obvious enhanced. Multi‐scale viscoelastic models of SMPC were established. Surface buckling behaviors of SMPC after U‐bending load were revealed. [ABSTRACT FROM AUTHOR]

Body‐temperature responsive shape memory polymers (SMPs) attract a lot of attention with the application in biomedicine. Multiple SMPs regulate the response temperature through the proportion of their stationary and reversible phases by changing the molecular weight of the polymer or the components of the composite. Herein, a crosslinking reaction of trans‐polyisoprene (TPI) and polycaprolactone (PCL) initiated by benzoyl peroxide gave a SMP of TPI/PCL, whose shape memory property is realized by stage‐division crystallization zone. Under the fixed ratio of TPI:PCL, the crystallization performance of TPI/PCL is controlled by the crosslinking density. The response temperatures of the components in TPI/PCL are selected for the stage‐division crystallization zone, making excellent shape memory performance at corresponding response temperatures. For the further achievement in controllable response temperature within a certain range, the relationship model between crosslinking density and response temperature is established, obtaining the customizable response temperature ranging 37–55 °C. The presented facile regulation method for response temperature will provide a new idea for the SMPs development. [ABSTRACT FROM AUTHOR]

Covalent adaptable networks (CANs), leveraging the dynamic exchange of covalent bonds, emerge as a promising material to address the challenge of irreversible cross‐linking in thermosetting polymers. In this work, we explore the introduction of a catalyst‐free and associative C=C/C=N metathesis reaction into thermosetting polyurethanes, creating CANs with superior stability, solvent resistance, and thermal/mechanical properties. By incorporating this dynamic exchange reaction, stress‐relaxation is significantly accelerated compared to imine‐bond‐only networks, with the rate adjustable by modifying substituents in the ortho position of the dynamic double bonds. The obtained plasticity enables recycle without altering the chemical structure or mechanical properties, and is also found to be vital for achieving shape memory functions with complex spatial structures. This metathesis reaction as a new dynamic crosslinker of polymer networks has the potential to accelerate the ongoing exploration of malleable and functional thermoset polymers. [ABSTRACT FROM AUTHOR]

Stimuli‐responsive photonic crystals with patterned microstructures are of great interest in developing reconfigurable nano‐optical devices. Leveraging unconventional all‐room‐temperature shape memory efforts and spatially resolved photopolymerization, herein, a facile method for micropatterning stimuli‐responsive photonic crystals is reported. Macroporous shape memory polymer (SMP) photonic crystals fabricated by colloidal templating can be deformed by cold programming, triggering the disappearance of their original structural colors. Exposure of the deformed samples to UV light through a photomask selectively disables the shape memory capabilities in the UV‐exposed regions. Hidden micropatterns defined by the photomask can be revealed by exposing the colorless SMP films to ethanol vapor, which triggers the shape memory recovery of the "memorized" ordered microstructures and the corresponding structural colors. Extensive nanoindentation experiments indicate that the exposure to UV light increases the crosslinking density and enhances the elastic modulus and toughness of the exposed regions by a factor of ≈2.0 and ≈5.2, respectively. Due to the formation of these extra crosslinks in the deformed configuration, they prevent normal shape memory behavior where the strained polymer chains rearrange from the temporary to permanent configuration when triggered by an external stimulus. This simple micropatterning technology can enable multistimuli‐responsive reconfigurable nanophotonic devices and chromogenic anticounterfeiting labels. [ABSTRACT FROM AUTHOR]

This study reports intrinsic multimodal memristivity of a nonconjugated radical polymer with ambient stability. Organic memristive devices represent powerful candidates for biorealistic data storage and processing. However, there exists a substantial knowledge gap in realizing the synthetic biorealistic systems capable of effectively emulating the cooperative and multimodal activation processes in biological systems. In addition, conventional organic memristive materials are centered on conjugated small and macromolecules, making them synthetically challenging or difficult to process. In this work, we first describe the intrinsic resistive switching of the radical polymer that resulted in an exceptional state retention of >105 s and on/off ratio of >106. Next, we demonstrate its bimodal cooperative switching, in response to the proton accumulation as a biological input. Last, we expand our system toward an advanced in-sensor computing system. Our research demonstrates a nonconjugated radical polymer with intrinsic memristivity, which is directly applicable to future electronics including data storage, neuromorphics, and in-sensor computing. [ABSTRACT FROM AUTHOR]

In this study, we investigate the fabrication of ambient room temperature responsive shape memory polyurethane (SMPU)‐coated fabric using a simple dip coating method, aiming to enhance the shape memory response of smart textiles. Two SMPU were synthesized using different chain extender 1,4 butanediol (BDO‐SMPU) and polyethylenimine (PEI‐SMPU). Critical parameters such as SMPU concentration, dwell time, and coating solution temperature are optimized to ensure exceptional shape memory performance while also maintaining the fabric's handle, comfort, and durability. We determined that PEI‐SMPU/Cotton fabric exhibits superior memory performance, with a 90.2% shape recovery at a 1% PEI‐SMPU concentration. Conversely, BDO‐SMPU fabric demonstrated a 75.8% shape recovery under different conditions (10% SMPU concentration, 50°C solution temperature). Furthermore, shape recovery is influenced by programming temperature and load; at 35°C and 10 N load, PEI‐SMPU/Cotton significantly outperforms BDO‐SMPU/Cotton, showing about 20% improvement in shape recovery. This study indicates that modifying SMPU from BDO‐SMPU to PEI‐SMPU can notably enhance shape recovery performance at 35°C, marking a significant advancement in human body temperature responsive smart fabric technology. [ABSTRACT FROM AUTHOR]

The utilization of leather waste (LW) in a polyurethane (PU) matrix makes a smart and novel shape stable phase change material (SSPCM). This is essential for sustainability as it reduces landfill waste after use. The PU is synthesized in bulk with a 90% yield, using biodegradable polycaprolactone diol and bio‐based polyol (castor oil), along with tolylene‐2,4‐diisocyanate. PL and PLG composites are prepared by blending of constituent components PU (P), LW (L), and poly(glycidyl methacrylate) (PGMA, G), as specified by their code names. Role of LW (hydrogen bonding and chemical crosslinking) and morphology are elucidated by FTIR and SEM, respectively. Self‐healing time (2 h), shape fixity ratios (Rf) (PL: 60–80% and PLG: 60–70%) and shape recovery ratios (Rr) (100% for both) are determined at 60°C. PLG displays faster shape recovery in water (<30 s) compared to air (>300 s). Shape stability and thermal properties of the SSPCM are examined using the temperature responsive leakage study, TGA, and DSC. This research introduces a new approach for using leather waste (LW) in SSPCM, with self‐healing and 100% Rr. This material may find application where SSPCM with high durability and flexibility is essential such as textile and footwear materials. [ABSTRACT FROM AUTHOR]

Thermal-responsive polymers have applications in smart devices, packaging materials, sensing structures, and smart grippers. On the other side, 3D printing of smart materials (4D printing) enables printing complex structures for specific applications. Low strength and high cost are two major problems with shape memory polymers. In the present study, shape-memory polyurethane (SMPU) and polylactic acid (PLA) blends were obtained, mechanical and shape recovery characteristics were obtained experimentally. 3D printable filaments of SMPU, PLA and SMPU/PLA blend were obtained from a twin-screw extruder, and required test specimens were printed and characterized. Flexural tests of SMPU/PLA blends were compared with pure SMPU for repetitive cycles. The present study shows improved results in mechanical properties with a limited loss in shape recovery by blending SMPU with PLA. Further, the present study gives a feasible future path to work on shape memory and conventional polymer blends. [ABSTRACT FROM AUTHOR]

Shape memory polymers are smart materials that remember their original shape and respond to external stimuli. They have tremendous applications in engineering and bio-medical fields. Having lower mechanical strength and high cost opens the scope to work on creating certain structures as a combination of conventional and shape memory polymers. Conventional and shape memory sandwich structures are suitable for working with various material combinations. The present study deals with developing 4D-printed conventional and shape memory sandwich structured combinations to understand their mechanical, shape memory, and failure phenomena. The present study showed the feasibility of using such combinations with improved mechanical properties with a small reduction in shape recovery. Further, the present study showed the delamination of conventional and shape memory polymer layers after a few cycles of shape recovery when subjected to severe bending deformation. [ABSTRACT FROM AUTHOR]

[Display omitted] 4D printing combines the typical 3D printing with "smart materials", allowing 3D printed materials to undergo a structural change over time. Since its original concept was first introduced in 2013, 4D printing became an innovative research that has received more attention from scientists in different fields. This review summarizes the progress achieved in 4D printing technologies and their associated materials. First, the technology and process of 4D printing are overviewed, and then the structure and properties of smart materials utilized in 4D printing are analyzed in depth, including metamaterials, shape memory materials, hydrogels, and self-healing polymers. We systematically illustrate the morphing mechanisms of the 4D printed smart materials, and then critically discuss the stimuli that can trigger transformation in the 4D printed smart materials, including heat, light, moisture, pH, electric current, and magnetic field. For 4D printed smart materials, all the changes programmed in the materials follow a mathematical model that allows scientists to predict and design the desired behaviors of the structures, using parameters such as the material distribution and the spatial gradients of the metric tensor. We finally conclude with the discussion of future challenges and opportunities for this ever-growing technology. Overall, 4D printing can create dynamic structures programmed to be responsive to external stimuli in the environment, widening its use in a myriad of applications such as rapid prototyping, electronics, biomedicine, soft robotics, self-assembly structures, smart sensors, and dynamic actuators. [ABSTRACT FROM AUTHOR]

Stroke is the second result for death and ischemic stroke constitutes most of all stroke cases. Ischemic stroke takes place when blood clot or embolus blocks cerebral vessel and interrupts blood flow, which often leads to brain damage, permanent disability, or death. There is a 4.5‐h (golden hour) treatment window to restore blood flow prior to permanent neurological impairment results. Current stroke treatments consist mechanical system or thrombolytic drug therapy to disrupt or dissolve thrombus. Promising method for stroke treatment is mechanical retrieving of thrombi employing device deployed endovascularly. Advent of smart materials has led to research fabrication of several minimally invasive endovascular devices that take advantage of new materials capabilities. One of these capabilities is shape memory, is capability of material to store temporary form, then activate to primary shape as subjected to stimuli. Shape memory polymers (SMPs) are employed as good materials for thrombectomy device fabrication. Therefore, current review presents thrombectomy device development and fabrication with SMPs. Design, performance, limitations, and in vitro or in vivo clinical results of SMP‐based thrombectomy devices are identified. Review also sheds light on SMP's future outlook and recommendations for thrombectomy device application, opening a new era for advanced materials in materials science. [ABSTRACT FROM AUTHOR]

Highlights High temperature shape memory polymers (HT‐SMPs) have great utilization in self‐deployable hinges/morphing structures for space/aerospace, and high‐temperature sensors/actuators for electronics. However, HT‐SMPs have many drawbacks, such as low stiffness, strength, thermal stability, and dynamic mechanical properties. This work aims at improving these properties of highly utilized space grade HT‐SMP, PEKK (polyether ketone ketone), by reinforcing it with low‐cost carbon fibers (CFs), and developing its composite via additive manufacturing. The additively manufactured CF/PEKK composites are annealed at 200 °C (CF/PEKK‐A200) and 250 °C (CF/PEKK‐A250), and for the first time, investigated for shape memory effect (SME). The shape fixity and the shape recovery of the CF/PEKK‐UNA (un‐annealed), CF/PEKK‐A200, and CF/PEKK‐A250 are noted to be 95.97%, 88.95%, and 86.40%, and 88.70%, 92.70%, and 95.19%, respectively with a significant weight saving potential of ⁓21%. Dispersion of CFs in PEKK and suitability of processing parameters (blending, extrusion, and 3D printing) are confirmed through scanning electron microscopy (SEM). Thermal degradation temperature (Td$$ {T}_d $$) of the printed CF/PEKK composite (⁓568 °C) is found to be ⁓3.5% higher than PEKK (⁓549 °C). CF/PEKK‐A250 exhibited the highest storage modulus (4438.23 MPa), ~158% higher than PEKK (1722.3 MPa), while CF/PEKK‐A200 demonstrated the highest tensile modulus (10.9 GPa), which is 138.5% higher than PEKK (4.57 GPa) and 312.88% higher than CF/PEKK‐UNA (2.64 GPa). Moreover, CF/PEKK‐A200 exhibited 237.46%, 138.51%, 127.08%, 61.48%, 32.93%, and 50.35% higher tensile modulus than PEEK, PEKK, PEK, CF/PEK, CF/PEEK, and CF/PEKK composites, respectively, showing great potential to replace them. Printed CF/PEKK composites are investigated for shape memory behavior. The printed composites exhibited outstanding shape memory properties. Printed‐A200 exhibited 138.51% enhanced tensile modulus than pure PEKK. Also, the printed‐A200 showed 313% enhanced modulus than printed‐UNA. Td$$ {T}_d $$ (568 °C) of the printed composites is found ⁓4% greater than pure PEKK. [ABSTRACT FROM AUTHOR]

Imprint lithography is one of the most used techniques for fabricating microstructures, owing to its high efficiency in both costs and time. However, imprinting has limited feasibility in realizing complex microstructures due to difficulties arising from the inherent limitations in the demolding process. Herein, a facile method is demonstrated for fabricating closed‐loop reentrant topographies with microscale meshes through a combination of imprint lithography and shape memory polymer (SMP). The mesh structure imprinted onto the pre‐pressed SMP pillar array can be elevated by utilizing the form‐switchable property of SMP to fabricate suspended micromesh. Suspended micromesh is fully supported by restored SMP micropillar array, exhibiting a closed‐loop shape that cannot be achieved with conventional imprint lithographic methods. Also, by the nature of reentrant geometry, liquid‐repellency can be realized even for liquids with a lower surface tension than water, offering numerous applications in self‐cleaning, droplet manipulation, and antifouling. Various liquid‐repellent performances of the fabricated suspended micromesh are investigated and compared to the theoretical expectations for a non‐wetting structure, confirming the successful establishment of reentrant topography in the fabricated structures. The proposed lithographic technique can be broadly utilized not only for liquid‐repellent surfaces but also for the fabrication of various functional structures. [ABSTRACT FROM AUTHOR]

Aiming to endow natural minerals with fast, high-sensitivity, and controllable smart light, humidity, solvent and temperature responsiveness, a novel ceramic clay and cucurbituril (CB) guest-host system (MVCB) inspired by nature was self-assembled and rearranged via an ingenious and simple design successfully. For the first time, the multi-functional MVCB not only displayed a high intelligent multi-stimuli responsiveness as light, humidity, solvent, and temperature switches, but also had multiple selective molecular recognition responses because of different organic vapor with CB and asymmetrical bilayer clay. For instance, due to the factors of guest-host and slow release, the average response speed of self-assembled shuffling the MVCB in methanol was as high as 108°/s compared with bilayer film without CB (20°/s). Besides, the MVCB exhibited controllable swift movement and was bending for grabbing three times its own weight. Moreover, the ultra-wide operating temperature of the MVCB from was ranging −196 to 300 °C under extreme condition. More interestingly, the MVCB presented a unique and compliable self-driven, smart switch, shape memory, environmental awareness and soft robotic gripper owing to the asymmetrical swelling and supramolecular of the CB. This work not only brings a simple, cost-effective, large-scale, and efficient strategy for multi-functionalized natural minerals materials, but also opens potential applications for intelligent response, extremely resistant substances, energy conversion and soft robotics. [ABSTRACT FROM AUTHOR]

Water-triggered shape memory polymers (SMPs) have been extensively studied for biomedical applications due to their advantages of non-thermal actuation capability. However, few studies have been carried out to explore the working principle of shape recovery onset, which is essentially determined by the complex reactions between polymer macromolecules and water molecules. In this study, we developed a phase separation model to describe the dynamic glass transition in water-triggered SMPs. Based on the phase transition theory, dense and dilute phase separations of polymer macromolecules can be achieved when the dynamic diffusions of water molecules in the SMPs undergo dehydration and absorption processes, respectively. Then, the dynamic glass transition is resulted from the dehydration and absorption of water molecules, leading to the dense and dilute phases in the SMPs. Therefore, a free-energy equation has been developed to characterize the recovery onset, in which the mixing free energy and elastic free energy are originated from the Flory–Huggins solution theory and phase separation model, respectively. Moreover, the glass transition and its connection to shape recovery behaviors, i.e. recovery ratio, relaxation time and dynamic mechanical modulus, have also been investigated, according to the Fick's diffusion law. Meanwhile, onset of programmable recovery has been explained by the dynamic phase separation, based on the transpiration theory and permeability model. Finally, the proposed model is verified using the experimental results reported in the literature. This study is expected to provide a fundamental approach to formulate the constitutive relationship between the dynamic phase separation and programmable recovery onset in the water-triggered SMPs. [ABSTRACT FROM AUTHOR]

This paper evaluates the design and fabrication of a thermoplastic polyurethane (TPU) shape memory polymer (SMP) using fused deposition modeling (FDM). The commercially available SMP filament was used to create parts capable of changing their shape following the application of an external heat stimulus. The characterization of thermal and viscoelastic properties of the SMP TPU revealed a proportional change in shape fixity and recovery with respect to heating and cooling rates, as well as a decreasing softening temperature with increasing shape memory history due to changes in the polymer microstructure. Inspired by the advancements in 3D and 4D printing, we investigated the feasibility of creating multi-material lattice structures using SMP and another thermoplastic with poor adhesion to TPU. A variety of interlocking lattice structures were evaluated by combining SMP with another thermoplastic that have poor adhesion with TPU. The tensile strength and failure modes of the fabricated multi-material parts were compared against homogenous SMP TPU specimens. It was found that the lattice interface failed first at approximately 41% of the ultimate strength of the homogenous part on average. The maximum recorded ultimate strength of the multi-material specimens reached 62% of SMP TPU's ultimate strength. These characterizations can make 4D printing technology more accessible to common users and make it available for new markets. [ABSTRACT FROM AUTHOR]

Liquid crystalline polymers (LCPs) represent a distinct class of materials that have garnered significant interest for their utilisation in diverse industrial and engineering applications. A prominent attribute of LCPs is their stimuli‐responsiveness. These materials can undergo deformation and subsequently recover their original shapes when subjected to external stimuli such as heat, light, and electromagnetic fields. The molecular structure of LCPs consists of mesogens and flexible tails, mirroring the fundamental molecular mechanism found in shape memory polymers. This characteristic positions LCPs as promising materials for shape memory applications. This article provides a comprehensive review of LCPs, focusing on their various forms of stimuli‐responsiveness. In addition, it delves into the application of additive manufacturing and machine learning technologies in the context of shape memory LCPs. Finally, the article concludes by exploring the critical applications of LCPs as shape memory materials. [ABSTRACT FROM AUTHOR]

The nanocomposites of polythiourethane (PTU) with Fe3O4 were fabricated via an isocyanate-free approach. The nanocomposites simultaneously had the reprocessing, shape memory and photothermal properties. First, a linear PTU carrying a plethora of thiol groups was synthesized via the ring opening polyaddition between a bicyclic trithiocarbonate and a poly (propylene oxide) diamine. In the meantime, the surfaces of Fe3O4 nanoparticles were functionalized with thiol groups. Second, the co-crosslinking between the linear PTU and the thiol-functionalized Fe3O4 was performed via the coupling of thiol radicals with a radical initiator. Notably, the nanocomposites of PTU with Fe3O4 were successfully obtained with the fine dispersion of Fe3O4 nanoparticle in PTU matrix. Compared to control PTU, the nanocomposites displayed the improved thermomechanical properties. More importantly, the nanocomposites had reprocessing properties. The dynamic exchange of disulfide bonds is responsible for the reprocessing behavior. Owing to the crosslinking with disulfide bonds, PTU had shape memory properties. Notably, the incorporation of Fe3O4 nanoparticles was capable of improving the shape memory properties. In addition, the nanocomposites displayed the photothermal properties with the incorporation of Fe3O4 nanoparticles. The photothermal conversion behavior can be utilized to trigger the shape recovery of the nanocomposites under near-infrared light irradiation and in a non-contact fashion. [ABSTRACT FROM AUTHOR]

Intelligent materials derived from green and renewable bio‐based materials garner widespread attention recently. Herein, shape memory polyurethane composite (PUTA/Fe) with fast response to near‐infrared (NIR) light is successfully prepared by introducing Fe3+ into the tannic acid‐based polyurethane (PUTA) matrix through coordination between Fe3+ and tannic acid. The results show that the excellent NIR light response ability is due to the even distribution of Fe3+ filler with good photo‐thermal conversion ability. With the increase of Fe3+ content, the NIR light response shape recovery rate of PUTA/Fe composite films is significantly improved, and the shape recovery time is reduced from over 60 s to 40 s. In addition, the mechanical properties of PUTA/Fe composite film are also improved. Importantly, owing to the dynamic phenol–carbamate network within the polymer matrix, the PUTA/Fe composite film can reshape its permanent shape through topological rearrangement and show its good NIR light response shape memory performance. Therefore, PUTA/Fe composites with high content of bio‐based material (TA content of 15.1–19.4%) demonstrate the shape memory characteristics of fast response to NIR light; so, it will have great potential in the application of new intelligent materials including efficient and environmentally friendly smart photothermal responder. [ABSTRACT FROM AUTHOR]

Implementing sustainable crop protection practices is crucial to protect global harvests and ensure high-quality food supplies. While priming is an established method in seed production for the fortification of plants against various stresses, it is not yet a standard practice in transplant cultivation. Thus, we evaluated the long-term effects of thermopriming—a heat-based priming technique—on the growth, development, and fruit yield of tomato plants. Following a recovery period of about six weeks for thermoprimed plants without stress inducers, we subjected them to subsequent salt stress to ascertain the persistence of the priming effects. Additionally, we compared the efficacy of thermopriming with benzothiadiazole (BTH), a chemical elicitor, in enhancing plant resilience to abiotic stress. While BTH application negatively impacted both plant growth and fruit health, thermopriming showed no such adverse effects on these parameters. Instead, thermopriming initially enhanced the plant defense mechanisms by increasing the accumulation of protective phenols and flavonoids in the leaves. Interestingly, while thermopriming did not alter the response to salt stress, it notably strengthened the overall resilience of the plants. Our findings underscore both the potential and temporal constraints of thermopriming memory. Nonetheless, primed plants exhibited temporarily increased stress tolerance, offering a means to safeguard the offspring. [ABSTRACT FROM AUTHOR]

Smart materials that respond to external stimuli are useful for applications ranging from artificial skin to sensing to cosmetics. Inspired by natural phenomena (self‐healing, shape memory, and shrinking), this work develops a novel smart bio‐composite using sustainable polyurethane (PU) and sugarcane bagasse (SB) waste without using a solvent. PU is synthesized using polycaprolactone (PCL) diol, castor oil (CO) as a polyol, and isophorone diisocyanate (IPDI) as diisocyanate. Composites are prepared using PU and SB in the presence and absence of poly(acrylic acid) (PAA) and are denoted as PBA and PB, respectively. TGA and DSC analysis indicate the broad (−68.4 °C to 192 °C) thermal stability of these materials. PBA and PB composites exhibited relatively fast (20–30 min) self‐healing and high shape fixity ratio (Rf) (70–83%), and shape recovery ratio (Rr) (82–100%) at 60 °C in the air. Furthermore, PBA shows hot water‐responsive rapid 100% shape recovery and also exhibits thermoresponsive shrinkage properties like human skin. PBA lifts a material 13.3±2 % of its original length by utilizing its thermoresponsive shrinking property. These inexpensive materials with self‐healing, shape recovery, high thermal stability, and thermo‐responsive properties are attractive and may be useful in artificial skin, sensor, and coating applications. [ABSTRACT FROM AUTHOR]

Shape memory polymers (SMPs) undergo changes between arbitrary shapes and programmed shapes upon exposure to specific stimulus, allowing them to restore their original shape. All kinds of external stimuli have a threshold to change the shape of the SMP. Especially, for the thermal type SMP, the critical temperature for shape restoration is typically near the glass transition temperature (Tg). In this study, the controllability of the restoration temperature is analyzed by adjusting the Tg of the polymer using Norland Optical Adhesive 63, which can be cured with UV irradiation. By varying the ambient temperature from 20 to 120 °C during UV exposure, Tg changes ranging from 35.84 to 50.50 °C are obtained, with corresponding changes in restoration temperature. As a practical application, a thermal‐activated SMP dry adhesive is developed with programmable Tg and switchable adhesion. The fabricated SMP dry adhesive exhibited strong adhesion to substrates with various surface roughness. Additionally, the shape memory effect allowed for easy detachment through shape recovery, and different adhesive performances at different temperatures are achieved by programming various Tg values. Moreover, the simple manufacturing process of the SMP dry adhesive is confirmed to be suitable for continuous fabrication processes based on roll‐to‐roll methods. [ABSTRACT FROM AUTHOR]

Shape memory composites now have a wide range of applications in aerospace, medical devices, and smart structures. Seven graphene‐carbon oxide/glass fiber (GO‐CF/GF) hybrid reinforced shape memory composites were prepared using vacuum infiltration hot pressing system (VIHPS) and the shape memory properties of the materials were investigated in 100°C test. By comparing and analyzing the microstructure and shape memory properties of composites containing different volume fractions of GFs, the mechanism of the influence of different hybrid contents of GFs on the organizational properties and shape memory properties was investigated. The results show that when the reinforcement of the composites were all carbon fibers, the composites had the largest elasticity modulus, harder material and the fixation rate of 77.15%, the recovery rate of 95.17%, the porosity of 0.80% and the shape recovery force of 7.98 N. When the reinforcement of the composites were glass fibers, the composites had the smallest elasticity modulus, softer material and the fixation rate of 94.89%, the recovery rate of 77.21%, the porosity of 13.56% and the recovery force of 2.28 N. The results of this test can lay a foundation for subsequent research on fibers with different mixing ratios. Highlights: The GO‐CF/GF/EP prepared by VIHPS has excellent shape memory properties.Fiber hybrid ratio affects the composite's porosity and its properties.Fiber hybrid ratio affects the composite's shape fixation, recovery, and memory force.The shape fixation of G6 decreases the lowest with test cycles.Carbon fiber content changes the zero‐stress plane of GO‐CF/GF/EP. [ABSTRACT FROM AUTHOR]

A dual‐responsive shape memory polymer, inspired by the heliotropic behavior of sunflowers, holds promise for innovative research, amalgamating the distinctive traits of shape memory polymers with nature's sunflower dynamics. In this investigation, we crafted a heat and light dual‐responsive shape memory polymer through liquid crystal display 3D printing technology, employing a meticulously formulated resin composition. The resin comprised epoxy acrylate as an oligomer, hydroxyethyl methacrylate as a monomer, and phenylic(2,4,6‐trimethylbenzoyl) phosphine oxide as a photo initiator. To confer light responsiveness, graphene oxide particles were integrated into the polymer matrix, designed to selectively absorb light wavelengths and instigate the shape memory effect upon light exposure. The resultant shape memory polymer showcased exceptional mechanical robustness and manifested superior responsiveness to temperature and light stimuli. This light‐responsive shape memory polymer, drawing inspiration from sunflowers, presents numerous potential applications, such as transfer printing, as demonstrated. [ABSTRACT FROM AUTHOR]

Poly(ethylene terephthalate) (PET), extensively employed in bottles, film, and fiber manufacture, has generated persistent environmental contamination due to its non‐degradable nature. The resolution of this issue requires the conversion of waste PET into valuable products, often achieved through depolymerization into monomers. However, the laborious purification procedures involved in the extraction of monomers pose challenges and constraints on the complete utilization of PET. Herein, a strategy is demonstrated for the polymer‐to‐polymer upcycling of waste PET into high‐value biodegradable and programmable materials named PEXT. This process involves reversible transesterifications dependent on ester bonds, wherein commercially available X‐monomers from aliphatic diacids and diols are introduced, utilizing existing industrial equipment for complete PET utilization. PEXT features a programmable molecular structure, delivering tailored mechanical, thermal, and biodegradation performance. Notably, PEXT exhibits superior mechanical performance, with a maximal elongation at break of 3419.2 % and a toughness of 270.79 MJ m−3. These characteristics make PEXT suitable for numerous applications, including shape‐memory materials, transparent films, and fracture‐resistant stretchable components. Significantly, PEXT allows closed‐loop recycling within specific biodegradable analogs by reprograming PET or X‐monomers. This strategy not only offers cost‐effective advantages in large‐scale upcycling of waste PET into advanced materials but also demonstrates its enormous prospect in environmental conservation. [ABSTRACT FROM AUTHOR]

We have examined the influence of bump shape and bonding pressure on low-temperature electrical properties of indium bump connections including superconducting transition temperature, normal state resistance, and superconducting critical current. We describe our test structures, bonding process, and methods of characterization. At temperatures below 1 K, we observe critical currents greater than 70 mA for indium bump connections with a nominal bump size of 17 µm × 17 µm. [ABSTRACT FROM AUTHOR]

Purpose: The paper aims to fabricate shape memory composites using polylactic acid (PLA) matrix and graphite. Shape memory polymers are a promising family of materials for biomedical applications because of their favourable mechanical properties, fast reactions and good biocompatibility. For most SMPs, however, achieving controllable sequential shape change is challenging. Design/methodology/approach: In the present work, 4D printing technology is used to fabricate shape memory composites using polylactic acid (PLA) matrix and graphite. A comparative study of pure PLA and graphite's different weight % composition has been done. Findings: By carefully managing the deformation state, PLA with graphite shape memory composites produced controllable sequential deformation with an amazing shape memory effect. Surface morphology, thermal properties, melt flow index and shape recovery tests have all been carried out to assess the qualities of manufactured samples. Originality/value: This is a one-of-a-kind to fabricate shape memory composites using graphite and a PLA matrix. Thus, this research attempts to deliver the possible use of PLA/graphite composites fabricated using 4D printing in robotics and biomedical devices. [ABSTRACT FROM AUTHOR]

Thermo-responsive, biocompatible polyurethane (PU) with shape memory properties is highly desirable for biomedical applications. An innovative approach to producing wound closure strips using shape memory polymers (SMPs) is of significant interest. In this work, PU composed of polycaprolactone (PCL) and 1,4-butanediol (BDO) was synthesized using two-step polymerization. Palm oil (PO) was added to PU for enhancing the Young's modulus of the PU beyond the set criterion of 130 MPa. It was found that PU had the ability to crystallize at room temperature and the segments of individual PCL and BDO polyurethanes crystallized separately. The crystalline domains and hard segment of PU greatly affected the tensile properties. The reduction of crystalline domains by the addition of PO and deformation at the higher melting temperature of the crystalline PCL polyurethane phase improved the shape fixity and shape recovery ratios. The new irreversible phase, raised from the permanent deformation upon stretching at the between melting temperature of the crystalline PCL and BDO polyurethanes of 70 °C, resulted in a decrease in shape fixity ratio after the first thermomechanical stretching–recovering cycles. The demonstration of PU as a wound closure strip showed its efficiency and potential until the surgical wound healed. [ABSTRACT FROM AUTHOR]

Thermoresponsive shape memory polymers (SMPs) have garnered increasing interest for their exceptional ability to retain a temporary shape and recover the original configuration through temperature changes, making them promising in various applications. The SMP shape change and recovery that happen due to a combination of mechanical loading and appropriate temperatures are related to its particular microstructure. The deformation process leads to the formation and growth of micro-cracks in the SMP structure, whereas the subsequent heating over its glass transition temperature Tg leads to the recovery of its original shape and properties. These processes also affect the SMP microstructure. In addition to the observed macroscopic shape recovery, the healing of micro-crazes and micro-cracks that have nucleated and developed during the loading occurs. Therefore, our study delves into the microscopic aspect, specifically addressing the healing of micro-cracks in the cyclic loading process. The proposed research concerns a thermoplastic polyurethane shape memory polymer (PU-SMP) MM4520 with a Tg of 45 °C. The objective of the study is to investigate the effect of the number of tensile loading-unloading cycles and thermal shape recovery on the evolution of the PU-SMP microstructure. To this end, comprehensive research starting from structural characterization of the initial state and at various stages of the PU-SMP mechanical loading was conducted. Dynamic mechanical analysis (DMA), differential scanning calorimetry (DSC), wide-angle X-ray scattering (WAXS) and scanning electron microscopy (SEM) were used. Moreover, the shape memory behavior in the thermomechanical loading program was investigated. The obtained average shape fixity value was 99%, while the shape recovery was 92%, which confirmed good shape memory properties of the PU-SMP. Our findings reveal that even during a single loading-unloading tension cycle, crazes and cracks nucleate on the surface of the PU-SMP specimen, whereas the subsequent temperature-induced shape recovery process carried out at the temperature above Tg enables the healing of micro-cracks. Interestingly, the surface of the specimen after three and five loading-unloading cycles did not exhibit crazes and cracks, although some traces of cracks were visible. The traces disappeared after exposing the material to heating at Tg + 20 °C (65 °C) for 30 min. The crack closure phenomenon during deformation, even without heating over Tg, occurred within three and five subsequent cycles of loading-unloading. Notably, in the case of eight loading-unloading cycles, cracks appeared on the surface of the PU-SMP and were healed only after thermal recovery at the particular temperature over Tg. Upon reaching a critical number of cycles, the proper amount of energy required for crack propagation was attained, resulting in wide-open cracks on the material's surface. It is worth noting that WAXS analysis did not indicate strong signs of typical highly ordered structures in the PU-SMP specimens in their initial state and after the loading history; however, some orientation after the cyclic deformation was observed. [ABSTRACT FROM AUTHOR]

Dithienylethene photoswitches with an aromatic π‐linker as the bridge between the two thiophene units are attractive starting materials for developing molecular solar thermal energy (MOST) storage systems, partly because the aromaticity of their ring‐open forms is a favorable feature with regard to the energy‐storage densities of their ring‐closed forms produced by photoinduced electrocyclization (photocyclization) reactions. At the same time, this typically leads to small barriers for their thermal cycloreversion reactions, which are not desirable in this context. Here, we use computational methods to show that this problem can be circumvented with polycyclic heteroaromatic π‐linkers. Specifically, through the tuning of the aromatic character of the individual rings of such a π‐linker (like indole or isoindole), it is shown to be possible to strike a delicate balance between the seemingly contrasting requirements of simultaneously achieving both a high energy‐storage density and a large cycloreversion barrier. Furthermore, this design is also found to provide for a quick and efficient photocyclization reaction, owing to the onset of excited‐state antiaromaticity in the π‐linker upon light absorption of the ring‐open form. Altogether, dithienylethenes with polycyclic heteroaromatic π‐linkers appear to have both thermal and photochemical properties suitable for further development into future MOST systems. [ABSTRACT FROM AUTHOR]

Near‐infrared (NIR)‐triggered shape memory hydrogels with promising mechanical strength hold immense potential in the field of biomedical applications and soft actuators. However, the optical and mechanical properties of currently reported hydrogels usually suffer from limited solubility and dispersion of commonly used photothermal additives in hydrogels, thus restricting their practical implementations. Here,, a set of NIR‐responsive shape memory hydrogels synthesized by polyaddition of diisocyanate‐terminated poly(ethylene glycol), imidazolidinyl urea (IU), and p‐benzoquinone dioxime (BQDO) is reported. The introduction of IU, a hydrogen bond reinforcing factor, significantly enhances the mechanical properties of the hydrogels, allowing for their tunable ranges of the ultimate tensile strength (0.4–2.5 MPa), elongation at break (210–450%), and Young's modulus (190–850 kPa). The unique hydrogels exhibit an intrinsic photothermal effect because of the covalently incorporated photothermal moiety (BQDO), and the photothermal supramolecular hydrogel shows controllable shape memory capabilities characterized by rapid recovery speed and high recovery ratio (>90%). This design provides new possibilities for applying shape memory hydrogels in the field of soft actuators. [ABSTRACT FROM AUTHOR]

Shape memory polymers (SMPs) are smart materials that enable to transform back to their original shape from the deformed state when subjected to external stimuli. They have shown great potential used as sensors and actuators in diverse applications. However, current research on SMPs primarily focuses on the utilization of a single source of stimuli (e.g., electricity, magnetism, light, etc.), which heavily restricts their potential in complex circumstances. In this study, a novel approach is developed to fabricate multi‐layer electrically/magnetically dual‐driven shape memory composites (ML‐EMSMCs) based on a magnetic field‐assisted digital light processing (MF‐DLP) 4D printing technique. The fabricated ML‐EMSMCs contain alternating high electric conductive layers (up to 5.37 × 10−3 S cm−1) and magnetic responsive layers (10.7 emu g−1), enabling Joule heat‐based and high‐frequency magnetic field induction‐based stimuli. Furthermore, the ML‐EMSMCs exhibited excellent shape memory behavior, good formability, and magnetic properties. The developed 4D printing techniques allows for the alignment of magnetic particles with a unidirectional magnetic field, significantly improving their shape recovery speed. The developed electrically/magnetically dual‐driven and photocurable SMP composites shed light on the development of actuators and sensors with multiple functionalities. [ABSTRACT FROM AUTHOR]

This article investigates the thermal, mechanical, and shape memory performances of 3D-printed polylactic acid (PLA), polyethylene terephthalate glycol (PETG), and their blends for potential applications in 4D printing. Differential Scanning Calorimetry reveals distinct glass transition temperatures for PLA-PETG blends, confirming their immiscibility. The integration of PETG alters the crystalline structure of PLA, shifting its behavior from brittle to ductile. This confirms PETG's function as an effective plasticizer. The tensile strength and Young's modulus are influenced by material composition and printing orientation. The results show that 75% PLA and 25% PETG blend demonstrated enhanced mechanical properties compared to other polymer blends. Shape memory experiments demonstrate exceptional fixity and recovery rates, reaching 100%, with the 75% PLA blend exhibiting outstanding performance across 15 cycles. These findings, coupled with insights into the impact of programming temperature, offer valuable perspectives for designing 4D-printed structures with shape memory attributes, unlocking innovative applications across diverse fields. [ABSTRACT FROM AUTHOR]

Polymeric vascular bioresorbable stents (BRSs) have been widely used for the treatment of coronary artery diseases. While additive manufacturing (AM) is changing the landscape of the healthcare sector by enabling the realization of patient‐specific stents with highly complex structures. There are, however, challenges associated with the use of polymeric BRS, particularly in‐stent restenosis (ISR), related to its poor mechanical properties. Therefore, the aim of this review is to provide an overview of recent advancements in the development of polymeric BRSs designed to meet both mechanical and biological requirements. First, biopolymers as well as shape memory polymers (SMPs) that are suitable for BRSs are highlighted and briefly described. Second, different types of designing structures of vascular stents in addition to introducing effective mechanical metamaterials, e.g., negative Poisson ratio (NPR) structures are addressed. Subsequently, AM methods currently being used to fabricate polymeric BRSs, are discussed and compared with conventional fabrication methods. Lastly, future directions for research are proposed in relation to existing challenges to the realization of a new generation of AM BRSs. Overall, this paper serves as a benchmark for future cardiovascular applications, especially in order to obtain clinically viable polymeric vascular stents by selecting suitable polymers, designs, and AM technologies. [ABSTRACT FROM AUTHOR]

This study evaluates the mechanical and shape-memory properties of PLA/Ni80Cr20 continuous wire composite materials. The samples were produced using an extrusion-based additive manufacturing (AM) process with in-melt simultaneous impregnation of metal wire, followed by 3D printing. The reinforced samples were fabricated using metal wires of 0.1 and 0.15 mm in diameter and 5 and 10% volume percentages. The maximum mechanical (tensile and flexural) properties were obtained in the reinforced samples with a 10% volume percentage of metal wire of 0.1 mm in diameter. The samples exhibited a maximum ultimate tensile strength of 116 MPa, a maximum tensile modulus of 11.7 GPa, a maximum flexural strength of 221 MPa, and a maximum flexural modulus of 17.8 GPa. This research used a novel method to investigate the shape-memory properties of PLA. By applying a potential difference to the samples, the heat generated by the metal wire was absorbed by the matrix polymer, which increased the temperature of the material. This increase in temperature resulted in a change in the samples' shape. The effect of voltage on the wire was investigated, and a voltage of 40 V was applied to the U-shaped samples with special fixtures to measure the shape recovery and shape stabilization percentage. Based on the final results, it can be deduced that 3D-printed composite materials, along with appropriate wire type, wire diameter, voltage, and uniform temperature distribution, can be used as shape-memory materials for a wide range of applications with desired temperature conditions, especially in cases where direct heat cannot be applied to the sample. [ABSTRACT FROM AUTHOR]

The objective of the present investigation is to synthesise and characterise the Cu-Al-Ag shape memory alloys with minor Mn addition. Synthesis of Cu-Al-Ag-Mn SMA was done by induction furnace and gravity die casting, with constant Ag/Mn ratio (5% Ag and 2% Mn), the aluminium composition is varied from 8% to 14%. The as-cast sample will be further subjected to thermo-mechanical treatment to produce a sheet which exhibits shape memory effect. This study is to determine the influence of Al content on shape memory characteristics, microstructure, and phase transformation temperatures. The phase fraction of β'1 increased from 56% to 67% along with subsequent reduction of γ1' phase fraction from 23% to 17%, which is essential for improvement of shape memory properties with increase of aluminium constituent. X-ray diffraction revealed that the crystalline size decreased 79 to 32 nm and lattice strains increased from 0.24% to 0.69% with increase of Aluminium. With an increase in aluminium content, the martensite transformation temperature decreased from 386°C to 246°C, and the shape memory effect increased from 81 to 90% strain recovery. The ability to control shape memory characteristics by changing Al composition will improve the scope for this alloy in various shape memory applications. [ABSTRACT FROM AUTHOR]

Widely applied aluminum alloys in ship hulls, underwater vehicles, and marine machinery experience severe corrosion in harsh marine environments. For corrosion protection of aluminum alloys, the most convenient, effective, and low-cost approach was the application of anti-corrosion coatings. Coatings possessing self-healing properties to spontaneously repair damages have emerged as a research focus for new types of coatings. In this study, focused on the indication and repair of anti-corrosion coating damages for aluminum alloys, the fluorescent aggregation-induced emission (AIE) composite probe, rhodamine-naphthalimide (RNI), was synthesized, and the composite polymer materials HPPA-SMPU containing 2-hydroxyphosphinoyl carboxylic acid-doped polyaniline and shape memory polyurethane were prepared. Coaxial electrospinning technology was introduced to combine the two and create the fibrous materials with the fiber wall constructed from HPPA-SMPU, encapsulating the interior RNI solution. The fibers were incorporated into the epoxy coatings. RNI exhibited water-triggered AIE, Al3+-CHEF (chelation-enhanced fluorescence), and pH-responsive fluorescent properties to indicate infrared laser-targeted points of coating damages. The photothermal properties of HPPA-SMPU caused localized heating of the damaged coatings, reaching the phase transition temperature of epoxy and SMPU, leading to softening, expansion, shape memory behavior, and healing of the coating damages. The self-healing approaches enhanced the protective performance of the coatings for aluminum alloys, showcasing and extending the development of synergistic and intelligent functions in novel self-healing coating technologies. [ABSTRACT FROM AUTHOR]

Stretchable and self-healable materials with excellent mechanical performance hold great promise for applications in flexible functional devices. Despite rapid developments, achieving high mechanical strength, extreme stretchability, and rapid self-healing capability in self-healing materials remains challenging. Here, inspired by the hierarchical structure and unique network of connective tissue, we fabricated a class of bionic nanocomposites with high stretchability, outstanding mechanical strength, and rapid self-healing ability by integrating the bottlebrush copolymer functionalized graphene oxide (BCP@GO) into a polyurethane (PU) matrix via in-situ polymerization. The bottlebrush copolymer (BCP) acted as a bond bridge for linking the GO nanosheets (noncovalent interaction) and PU chains (covalent and hydrogen-bond interaction). The covalent interactions were responsible for providing high mechanical strength, and the abundant hydrogen-bond-based cross-links realized extreme stretchability and rapid self-healing capability. The resultant BCP@GO/PU nanocomposite with only 0.5 wt.% GO loading exhibited excellent mechanical properties (tensile strength increased by 52.1%, up to 28.6 MPa; toughness increased by 70.8%, up to 256.9 MJ/m3; elongation at break increased by 12.8%, up to 1847.2%), exceptional rapid and efficient self-healing ability (~ 99% with 20 s NIR irradiation), as well as superior shape memory and recyclable capability. This study develops a new strategy for designing high-performance self-healing nanocomposites and unfolds broad application prospects in smart materials. [ABSTRACT FROM AUTHOR]

In the present study, the selection of suitable shape memory polymers (SMPs) to be used as the matrix‐phase material with various (In)organic filler materials to achieve the required optimum multi‐stimuli response in shape memory polymer composites (SMPC) systems is analyzed. The selection of these materials is based on their mechanical and physical properties as well as other underlying factors such as cost, availability, shape recovery rate, and aesthetic characteristics. In this study, the entropy method was applied to estimate the weightages of the various criteria while the gray relation analysis (GRA) and the technique for order preference by similarity to ideal solution (TOPSIS). Multi‐criteria decision‐making (MCDM) approaches have been used to rank the suitable matrix‐phase polymer materials for manufacturing shape memory polymer composites (SMPC) system. A total of eight alternative SMP matrix‐phase materials based on a set of nine criteria were analyzed and ranked. The proposed methodology and the result obtained thereof have been illustrated in detail. The results obtained from TOPSIS and GRA methods have been compared to conclude the effects of the material properties on the ranking and the selection of the SMP materials. Among all the eight alternatives considered, thermoplastic polyurethane (TPU) was found to be the best material in both the MCDM methods. The material cost, resistivity, % elongation, and hydrophobicity present the most influencing properties on the SMP material selection, whereas density presents no effect on the SMP matrix material selection. The robustness of the results for the comparative analysis was verified using TOPSIS methodology to validate its reliability. It was revealed that the TPU, polycarbonate, polypropylene, and epoxy‐resin/poly(lactic acid) are the most dominant matrix‐phase SMP material alternatives when a deviation in the entropy weights of the primary evaluation criteria is applied. The novelty of this study is the exploration and application of statistical MCDM methods of engineering material selection problems based on a set of decision criteria, which can be time‐consuming and costly while using experimental analysis methods. Highlights: SMPCs are applicable engineering materials thus making their research viable.SMPC systems can undergo various shape changes under external stimuli.Selection of matrix‐phase polymer is critical in achieving desired objectives.GRA and TOPSIS MCDM approaches have been applied in the selection process.TPU was found as the best material in both methods. [ABSTRACT FROM AUTHOR]