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Core-shell structures exhibit a number of distinct absorptive properties that make them attractive tools for use in a range of industrial contexts including pharmaceuticals, biotechnology, cosmetics, and food/agriculture. Several recent studies have focused on the development and fabrication of zein-based core-shell structures for a range of functional material deliveries. However, no recent review article has evaluated the fabrication of such core-shell structures for food-based applications. In this paper, we therefore survey current approaches to fabricating different zein-based platforms including particles, fibers, films, and hydrogels that have appeared in a variety of functionally relevant applications. In addition, we highlight certain challenges and future research directions in this field, thereby providing a novel perspective on zein-based core-shell structures. • The methods employed in zein-based core-shell structure synthesis and fabrication • Applications of zein-based core-shell from established to future development • Benefits and challenges for zein-based core-shell microstructures [ABSTRACT FROM AUTHOR]

The enhancement of antimicrobial wound dressings is of utmost importance in light of the escalating risk of antibiotic resistance caused by excessive antibiotic usage. Conventional antimicrobial materials eradicate pathogenic bacteria while impeding the proliferation of beneficial bacteria during the management of wound infections, thereby disturbing the equilibrium of the skin micro-ecosystem and engendering recurrent cutaneous complications. Lactobacillus rhamnosus (L.rha) is a probiotic that can inhibit the growth of certain pathogenic bacteria by secreting a large number of metabolites. In this paper, we synthesized a cross-linker (SPBA) with a boric acid molecule from succinic acid and 4-(bromomethyl)phenylboronic acid, which formed a boric acid ester bond with a diol on the natural polysaccharide sodium alginate (SA), and obtained a pH/reactive oxygen species (ROS) dual-responsive hydrogel (SA-SPBA) for loading L.rha to treat wound infections. The SA-SPBA@L.rha hydrogel improves the survival of L.rha during storage and has good injectability as well as self-healing properties. The hydrogel showed good biocompatibility, the antimicrobial effect increases in a dose-dependent manner, and it has a certain antioxidant and anti-inflammatory capacity, accelerating wound repair. The use of SA-SPBA@L.rha hydrogel provides a safe and effective strategy for the repair of skin wound infections. [ABSTRACT FROM AUTHOR]

The development of biopolymer-based filtration systems for water remediation applications is an extremely fascinating area of research. In this paper, we developed a biopolymer-based filtration system using sodium alginate (NaAlg) and carrageenan (Car) for the removal of the toxic cationic dye, methylene blue (MB). The membrane's properties were assessed using FTIR, TGA, UTM, FESEM, EDS, XRD, and water uptake, revealing commendable thermomechanical stability (5.79 MPa), good hydrophilicity, and compatibility. The experimental results further revealed that lambda Car/calcium alginate (λ-Car/CaAlg) exhibited superior dye rejection (100%) and flux (11.67 L m−2 h−1) compared to kappa Car/CaAlg (κ-Car/CaAlg) (99.22% and 11.19 L m−2 h−1) and plain alginate (CaAlg) (99.63% and 9.79 L m−2 h−1). The high MB rejection rate was attributed to the sieving mechanism and electrostatic interaction. A rejection rate of 100% was achieved at an initial MB concentration of 10 mg/L, pressure of 0.1 MPa, pH of 7, and temperature of 25°C. Furthermore, the hydrogel membranes demonstrated excellent recyclability over nine cycles, indicating their potential for water treatment applications. [ABSTRACT FROM AUTHOR]

Hydrogels have shown great potential for application in food science due to their diverse functionalities. However, most hydrogels inevitably contain toxic chemical cross-linking agent residues, posing serious food safety concerns. In this paper, a curcumin/sodium alginate/carboxymethyl chitosan hydrogels (CSCH) were prepared by self-assembly of two oppositely charged polysaccharides, carboxymethyl chitosan and sodium alginate, to form a three-dimensional network encapsulating curcumin for extending food shelf life. The network structure of the CSCH film confirmed by FTIR, XRD, and XPS was mainly formed by electrostatic interactions. The chemical stability of CSCH network encapsulated curcumin was 4.2 times greater than that of free curcumin, with excellent gas barrier, antimicrobial, antioxidant, and biosafety properties. It was found that CSCH films reduced dehydration, prevented nutrient loss, inhibited microbial growth, and lowered the respiration rate, which effectively maintained the quality of mango and prolonged its shelf-life up to 11 days. Notably, CSCH films possessed the properties of rapid recycling (10 mins) and biodegradability (53 days). This polysaccharide-based hydrogel film provides a viable strategy for the development of green and sustainable food packaging. [Display omitted] [ABSTRACT FROM AUTHOR]

After skin tissue trauma, wound infections caused by bacteria posed a great threat to skin repair. However, resistance to antibiotics, the current treatment of choice for bacterial infections, greatly affected the efficiency of anti-infection and wound healing. Therefore, there has been a critical need for the development of novel antimicrobial materials and advanced therapeutic methods to aid in skin repair. In this paper, rGO-PDA@ZIF-8 nanofillers were prepared by coating graphene oxide (GO) with dopamine (DA), followed by in situ growth of zeolite imidazolate framework-8 (ZIF-8). Using polyvinyl alcohol (PVA) and chitosan quaternary ammonium salt (CS) as matrix materials, along with polyethylene glycol (PEG) as a pore-forming agent, and rGO-PDA@ZIF-8 as an antimicrobial nano-filler, we successfully prepared rGO-PDA@ZIF-8/PVA/CS composite hydrogels with a directional macroporous structure using bidirectional freezing method and phase separation technique. This hydrogel exhibited excellent mechanical properties, good solubility and water retention capabilities. In addition, the hydrogel demonstrated excellent biocompatibility. Most notably, it not only exhibited excellent bactericidal effect against E. coli and S. aureus (99.1 % and 99.0 %, respectively) under the synergistic effect of intrinsic antibacterial activity and photothermal antibacterial, but also exhibited the ability to promote wound healing, making it a promising candidate for wound healing applications. [ABSTRACT FROM AUTHOR]

The enormous potential of multifunctional bilayer wound dressings in various medical interventions for wound healing has led to decades of exploration into this field of medicine. However, it is usually difficult to synthesize a single hydrogel with all the required capabilities simultaneously. This paper proposes a bilayer model with an outer layer intended for hydrogel wound treatment. By adding gelatin methacrylate (GelMA) and tannic acid (TA) to the hydrogel composition and using polyvinyl alcohol-carboxymethyl chitosan (PVA-CMCs) foam layer as supports, a photocrosslinkable hydrogel with an optimal formulation was created. The hydrogels were then examined using a range of analytical procedures, including mechanical testing, rheology, chemical characterization, and in vitro and in vivo tests. The resulting bilayer wound dressing has many desirable properties, namely uniform adhesion and quick crosslinking by UV light. When used against Gram-positive and Gram-negative bacterial strains, bilayer wound dressings demonstrated broad antibacterial efficacy. In bilayer wound dressings with GelMA and TA, better wound healing was observed. Those without these elements showed less effectiveness in healing wounds. Additionally, encouraging collagen production and reducing wound infection has a major therapeutic impact on wounds. The results of this study could have a significant impact on the development of better-performing wound dressings. [Display omitted] [ABSTRACT FROM AUTHOR]

The enormous potential of multifunctional bilayer wound dressings in various medical interventions for wound healing has led to decades of exploration into this field of medicine. However, it is usually difficult to synthesize a single hydrogel with all the required capabilities simultaneously. This paper proposes a bilayer model with an outer layer intended for hydrogel wound treatment. By adding gelatin methacrylate (GelMA) and tannic acid (TA) to the hydrogel composition and using polyvinyl alcohol-carboxymethyl chitosan (PVA-CMCs) foam layer as supports, a photocrosslinkable hydrogel with an optimal formulation was created. The hydrogels were then examined using a range of analytical procedures, including mechanical testing, rheology, chemical characterization, and in vitro and in vivo tests. The resulting bilayer wound dressing has many desirable properties, namely uniform adhesion and quick crosslinking by UV light. When used against Gram-positive and Gram-negative bacterial strains, bilayer wound dressings demonstrated broad antibacterial efficacy. In bilayer wound dressings with GelMA and TA, better wound healing was observed. Those without these elements showed less effectiveness in healing wounds. Additionally, encouraging collagen production and reducing wound infection has a major therapeutic impact on wounds. The results of this study could have a significant impact on the development of better-performing wound dressings. [Display omitted] [ABSTRACT FROM AUTHOR]

This paper presents the formation of a self-healing hydrogel prepared by carboxyethyl modification of chitosan and crosslinking with oxidized sodium alginate. Concurrently, the incorporation of Ca2+ facilitated the formation of "calcium bridges" through intricate coordination with carboxyl moieties, bolstering the attributes of the hydrogel. Various characterization methods, including scanning electron microscopy, texture analysis, and rheological measurements, demonstrated that the introduction of carboxyethyl groups resulted in a more compact hydrogel network structure and improved the hardness and elasticity. The addition of Ca2+ helped to further enhance the mechanical performance of the hydrogel and increase its thermal stability. Then, the adsorption capacity was also investigated, showing adsorption capacities of 46.17 mg/g methylene blue and 46.44 mg/g congo red for carboxyethyl chitosan/oxidized sodium alginate hydrogel, a four-fold increase for congo red versus chitosan/oxidized sodium alginate hydrogel. In addition, the adsorption behavior of CEC/OSA/2%Ca2+ hydrogel can be well described by pseudo-second-order kinetic model and Langmuir adsorption isothermal model. Compared to traditional hydrogels, CEC/OSA/2%Ca2+ hydrogel shows superior mechanical strength, enhanced thermal stability, and improved adsorption capacity, which can effectively adsorb not only methylene blue but also congo red. These advancements demonstrate our hydrogel's innovative properties. [Display omitted] [ABSTRACT FROM AUTHOR]

Tannic acid (TA) is a natural compound studied as the cross-linker for biopolymers due to its ability to form hydrogen bonds. There are different methods to improve its reactivity and effectiveness to be used as a modifier for biopolymeric materials. This work employed plasma to modify tannic acid TA, which was then used as a cross-linker for fabricating collagen/gelatin scaffolds. Plasma treatment did not cause any significant changes in the structure of TA, and the resulting oxidized TA showed a higher antioxidant activity than that without treatment. Adding TA to collagen/gelatin scaffolds improved their mechanical properties and stability. Moreover, the obtained plasma-treated TA-containing scaffolds showed antibacterial properties and were non-hemolytic, with improved cytocompatibility towards human dermal fibroblasts. These results suggest the suitability of plasma treatment as a green technology for the modification of TA towards the development of advanced TA-crosslinked hydrogels for various biomedical applications. The four stages of work described in the paper starting with the plasma-treatment of TA, characterization of the final product, fabrication of collagen-gelatin-TA-based hydrogels, and their general characterization. Graph was generated via Biorender.com. [Display omitted] [ABSTRACT FROM AUTHOR]

Bio-based materials are rapidly replacing synthetic materials owing to their significant biomedical applications, easy availability, nontoxicity, biodegradability and biocompatibility. Guar gum (GG) is a plant-derived biocompatible and biodegradable polymeric compound found abundantly in nature. It is a non-ionic, hydrophilic carbohydrate and is a cost-effective hydrocolloid polysaccharide considered as a wonderful representative of the new generation of plant gums. Various composites of guar gum with other polymers have been reported in last few decades and they are extensively used in different industries like food, textile, mining, petrochemical, paper and explosives etc. Easy availability, non-toxicity, eco-friendly and biodegradable nature of GG has made it ideal candidate for for drug delivery (DD) applications. GG based hydrogels, films, scaffolds and nanoparticles have been explored widely for their DD applications. These non-toxic DD carriers can be used for targeted drug delivery. This review article directs the current efforts and improvements on GG and GG-based materials to be used in DD. [Display omitted] • Gar gum; one of the cheapest source material of galactomannan • Physico-chemical properties of gar gum are reported. • An update on gargum based materials for drug deleivery appliactions [ABSTRACT FROM AUTHOR]

The healing of full-thickness skin defect has been a clinical challenge. Hydrogels with multiple functions inspired by extracellular matrix are expected to be used as wound dressing. In this paper, dopamine-grafted oxidized hyaluronic acid was blended with quaternary ammonium chitosan to form a composite functionalized hydrogel by enzyme-catalyzed cross-linking and Schiff base reaction. The hydrogel has convenient preparation, good biocompatibility, antibacterial and antioxidant, high adhesion and self-healing properties. The results in vivo show that the hydrogel can effectively close the wound and accelerate the speed of wound healing by up-regulating the expression of angiogenic protein and promoting the distribution of collagen deposition more uniform and regular. It is expected that this composite functionalized hydrogel dressing has great potential in wound regeneration. [ABSTRACT FROM AUTHOR]

The healing of full-thickness skin defect has been a clinical challenge. Hydrogels with multiple functions inspired by extracellular matrix are expected to be used as wound dressing. In this paper, dopamine-grafted oxidized hyaluronic acid was blended with quaternary ammonium chitosan to form a composite functionalized hydrogel by enzyme-catalyzed cross-linking and Schiff base reaction. The hydrogel has convenient preparation, good biocompatibility, antibacterial and antioxidant, high adhesion and self-healing properties. The results in vivo show that the hydrogel can effectively close the wound and accelerate the speed of wound healing by up-regulating the expression of angiogenic protein and promoting the distribution of collagen deposition more uniform and regular. It is expected that this composite functionalized hydrogel dressing has great potential in wound regeneration. [ABSTRACT FROM AUTHOR]

Most three-dimensional (3D) printed hydrogel exhibit non-idealized rheological properties in the process of direct ink writing and complicated curing. Therefore, accurate writability and convenient curing for 3D printed hydrogel remain a challenge. In this paper, we developed a typical 3D printed hydrogel which realized direct ink writing (DIW) at temperatures similar to human body. Silicon dioxide (SiO 2) and Gum Arabic (GA) formed the Bingham fluid to ensure shape stability. The rapid initiation system of potassium persulfat (KPS) and N,N,N′,N′ -tetramethylethylenediamine (TMEDA) allowed the 3D printed hydrogel precursor solution to transiently form a hydrophobic conjoined cross-linking network structure of acrylamide (AAM) and lauryl methacrylate (LMA) after printing, resulting in preferable mechanical properties. Hydrogel precursor solution showed better rheological properties with the nature of Bingham fluids, and achieved transient cross-linking at 30 °C for 10 s in the rheological test. A variety of 3D printed hydrogel with individual strain sensing properties are prepared as customizable sensor that could monitor significant strain signals within 0–20 % strain with high sensitivity. Moreover, they were discovered excellent temperature sensitivity over a wide operating range (0–80 °C). The 3D printing hydrogel sensors were expected to have broad application prospects in flexible wearable devices and medical monitoring. [ABSTRACT FROM AUTHOR]

Hydrogel microspheres stand out in drug delivery due to their small particle size, biocompatibility and good internal stability. In this paper, pH-sensitive hydrogels are prepared by microfluidic technology for targeted drug delivery in the small intestine. A coaxial dual-channel microfluidic chip is constructed. By analyzing the effects of flow rates and three fracture stages (Rayleigh-Plateau instability crushing stage, pressure difference crushing stage and shear force crushing stage) on the size of hydrogel microspheres, the optimal control stage of the microsphere size is determined (shear force crushing stage). Based on this, the accurate control model of the hydrogel microsphere size is proposed. In addition, based on the coaxial dual channel microfluidic chip, a monolayer hydrogel microcapsule loaded with Indometacin is prepared. The core-shell hydrogel microcapsules loaded with Indometacin are prepared by an improved coaxial three channel microfluidic chip. The swelling rates of both microcapsules in simulated intestinal fluid are significantly higher than those in simulated gastric fluid. The results of in vitro simulated release experiments show that the two hydrogel microcapsules basically do not release in simulated gastric juice. In simulated intestinal fluid, single-layer hydrogel microcapsules show rapid release, while core-shell hydrogel microcapsules showed slow release. In conclusion, the alginate-based hydrogel microcapsules have good stability and pH sensitivity, and are suitable for targeted drug delivery in the small intestine. [ABSTRACT FROM AUTHOR]

Bletilla striata has been used for thousands of years and shows the functions of stopping bleeding, reducing swelling, and promoting healing in traditional applications. For Bletilla striata, Bletilla striata polysaccharides (BSP) is the main active ingredient, exhibiting biological functions of anti-inflammatory, anti-oxidant, anti-fibrotic, immune modulation, anti-glycation, and so on. In addition, BSP has exhibited the characteristics of excipient such as bio-adhesion, bio-degradability, and bio-safety and has been prepared into a series of preparations such as nanoparticles, microspheres, microneedles, hydrogels, etc. BSP, as both a drug and an excipient, has already aroused more and more attention. In this review, publications in recent years related to the extraction and identification, biological activities, and excipient application of BSP are reviewed. Specifically, we focused on the advances in the application of BSP as a formulation excipient. We hold opinion that BSP not only needed more researches in the mechanisms, but also the development into hydrogels, nano-formulations, tissue engineering, and so on. And we believe that this paper provides a beneficial reference for further BSP innovation and in-depth research and promotes the use of these natural products in pharmaceutical applications. [ABSTRACT FROM AUTHOR]

Sustainable composite hydrogel materials with harsh environmental adaption and tolerance capability have received considerable interests but still remain as challenges. In this work, biomimetic strategy was adapted for construction of three-dimensional galactomannan (GM) hydrogels with intercalation of flexible polymer chains polyethyleneimine (PEI), biomacromolecules tannin acid (TA) and CeO2 nanoparticles (NPs). The hydrogels cross-linked with double-networks (DN) present not only pH-responsive water absorption property, but also boosted mechanical strength with highest toughness of 326 kJ/m3 and Young's modulus of 220 kPa. Self-healing and anti-freezing capabilities were revealed for the hydrogels by maintaining of fracture elongation (23 %) and fracture strength (250 kPa). TA, CeO2 NPs as well as the amide groups in PEI of the hydrogels introduced excellent bacterial prohibition performance on both Bacillus subtilis (B. subtilis) and Escherichia coli (E. coli). Also, due to the existence of the free ions, the hydrogels exhibited electric conductive properties, with wide-range high sensitivity and long-time conductive stability. In addition, various tensile strain degrees were related to the conductive resistance values, and the great recovery performance was proved by cyclic tensile-conductive tests for 3000 times. Therefore, the proposed GM-based hydrogels displayed great potentials as strain sensors that are adaptable and tolerant to various environmental conditions. [ABSTRACT FROM AUTHOR]

Local drug delivery has generated considerable interest due to its controlled and sustained drug release at the target site on demand. Nanoaggregate-incorporated composite hydrogels are desirable as local drug delivery systems; however, it is difficult to achieve sustained and controlled hydrophobic drug release and superior mechanical properties in one system. Herein, a "smart" composite hydrogel was synthesized by incorporating hemicellulose-based nanoaggregates into a double network consisting of alginate/Ca2+ and polyacrylic acid- co -dimethylaminoethyl methacrylate [P(AA-co-DMAEMA)]. Hemicellulose-based nanoaggregates were assembled from xylan-rich hemicellulose laurate methacrylate (XH-LA-MA) polymers and entrapped into the hydrogel framework via chemical fixation. Another composite hydrogel with physically embedded hemicellulose laurate (XH-LA) nanoaggregates was prepared as a comparison. Accordingly, covalently cross-linked XH-LA-MA nanoaggregates in hydrogels resulted in a denser pore structure and reinforced mechanical properties. Nanoaggregate diffusion analysis revealed that covalent bonding between the nanoaggregates and the hydrogel framework contributed to prolonged diffusion behavior. Curcumin (Cur)-loaded XH-LA-MA composite hydrogels enabled sustained Cur release in simulated body fluid and showed stimulus responsiveness toward ethylenediaminetetraacetic acid (EDTA) and/or glutathione (GSH). All the composite hydrogels were biocompatible, as verified by Cell Counting Kit-8 (CCK-8) assay against NIH/3T3 cells. These composite hydrogels hold great potential as a promising dosage form for biomedical applications. [Display omitted] • A composite hydrogel was synthesized by incoporating hemicellulose-based nanoaggregates into a double network. • Covalent bonding between nanoaggregates and the hydrogel framework contributed to enhanced mechanical properties. • Curcumin-loaded composite hydrogels showed sustained and controlled release behaviors. • The hydrogel-nanoaggregate composites were biocompatible for biomedical applications. [ABSTRACT FROM AUTHOR]

Inspired by the mussel, tannic acid (TA) was modified onto the surface of self-made cellulose nanofibrils (CNFs) to prepare TA@CNFs, which was introduced into borax crosslinked polyvinyl alcohol (PVA) to prepare PTC double-network hydrogel with self-healing properties. Through the comparative observation of TEM images and infrared spectra before and after tannic acid modification, the formation of TA@CNFs was proved. The introduction of TA@CNFs greatly increases the fracture stress of PTC hydrogel, which is more than 10 times higher than that of PVA hydrogel without TA@CNFs, and has high fracture strain (1723 %). Moreover, PTC hydrogel has the ability of rapid self-healing, which can heal to the original form within two minutes. In addition, the temperature response ability of PTC hydrogel makes it capable of reshaping. The self-adhesion ability of PTC hydrogel enables it to adhere to the human epidermis to detect motion signals, as sensitive and as stable as a flexible sensor. [Display omitted] [ABSTRACT FROM AUTHOR]

Pectin-crosslinked gum ghatti hydrogel (PGH) has been synthesized utilizing pectin and gum ghatti through an uncomplicated and inexpensive copolymerization method. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM-elemental mapping), Brunauer-Emmett-Teller (BET), and X-ray photoelectron spectroscopy (XPS) characterization techniques have been employed to determine various structural, chemical and compositional characteristics of fabricated PGH. Three different weight ratios (1:1, 2:1, or 1:2 for pectin and gum ghatti, respectively) were employed to synthesize three distinct types of PGH. Swelling studies has been done to determine the best ratios for PGH fabrication. PGH has been assessed as an adsorbent for the removal of malachite green dye from aqueous solutions. The effects of PGH dosage (100–400 mg/L), dye concentration (10–160 mg/L), pH (2–9 pH), adsorption time (0–480 min), and temperature (25–55 °C) has been examined through batch solutions. According to Langmuir isotherm analysis, the maximum adsorption capacity is 658.1 mg/g. By using pseudo-second-order kinetics and the Freundlich adsorption isotherm, the adsorption process could be well explained. After five consecutive cycles, PGH had an adsorption percentage of 86.917 % for the malachite green dye. It is safe for the environment and may be used to remove malachite green (MG) dye from aqueous solutions. [Display omitted] • Pectin-crosslinked gum ghatti hydrogel (PGH) synthesis using copolymerization • Study of physicochemical properties of PGH • PGH effectively adsorbed malachite green (MG) dye. • Showing a maximum capacity of 658.1 mg/g according to Langmuir isotherm analysis • Freundlich isotherm model fits well, indicating a heterogeneous adsorption process. [ABSTRACT FROM AUTHOR]

Electro-conductive hydrogels emerge as a stretchable conductive materials with diverse applications in the synthesis of flexible strain sensors. However, the high-water content and low cross-links density cause them to be mechanically destroyed and freeze at subzero temperatures, limiting their practical applications. Herein, we report a one-pot strategy by co-incorporating cellulose nanofiber (CNF), Poly pyrrole (PPy) and glycerol with polyvinyl alcohol (PVA) to prepare hydrogel. The addition of PPy endowed the hydrogel with good conductivity (∼0.034 S/m) compared to the no PPy@CNF group (∼0.0095 S/m), the conductivity was increased by 257.9 %. The hydrogel exhibits comparable ionic conductivity at −18 °C as it does at room temperature. It's attributed to the glycerol as a cryoprotectant and the formation of hydrated [Zn(H 2 O) n ]2+ ions via strong interaction between Zn2+ and water molecules. Moreover, the cellulose nanofiber intrinsically assembled into unique hierarchical structures allow for strong hydrogen bonds between adjacent cellulose and PPy polymer chains, greatly improve the mechanical strength (stress∼0.65 MPa, strain∼301 %) and excellent viscoelasticity (G'max ∼ 82.7 KPa). This novel PPy@CNF-PVA hydrogel exhibits extremely high Gauge factor (GF) of 2.84 and shows excellent sensitivity, repeatability and stability. Therefore, the hydrogel can serve as reliable and stable strain sensor which shows excellent responsiveness in human activities monitoration. • The flexible strain sensors based on PPy@CNF-PVA hydrogels were prepared by a facile one-pot strategy. • The sensors exhibited extremely high GF of 2.84 and shows excellent sensitivity, repeatability and stability. • The sensors could work at −18 °C without freezing and monitor human activities. [ABSTRACT FROM AUTHOR]

Lignocellulosic nanofibril (LCNF) is indispensable in numerous potential applications because of its unsurpassed quintessential characteristics. While it still remains a challenge to assemble LCNF in a facile and environmental economy-first manner. In this work, a simple and green one-step synthetic approach was reported to prepare a series of LCNF-containing versatile hydrogels using deep eutectic solvent (DES). In particular, the LCNF5% hydrogel (namely LCNF5%-gel) in this work perfectly integrated superior stretchability (∼643 %), and displayed a dramatically improved anti-swelling ability (25 %) compared to the control sample (neat DES hydrogel, 2252 %). Simultaneously, the LCNF5% hydrogel presented underwater adhesiveness and outstanding long-term low-temperature resistance (stable at −25 °C for a month). This novel multifunctional hydrogel, prepared by a facile and eco-friendly strategy, is potentially useful in wet adhesion or underwater applications. • Lignocellulose nanofibril was used to prepare multifunctional hydrogels. • This hydrogel was prepared with a one-step approach using deep eutectic solvent. • The hydrogel presented good anti-swelling and long-term low-temperature resistance. • The product can be potentially useful in wet adhesion or underwater applications. [ABSTRACT FROM AUTHOR]