Self‐strengthened hydrogel actuator based on the distribution of size‐differentiated PVAcrystallites

Soft tissues, such as muscle could autonomously grow through re‐alignment and/or ‐combination of collagen nanofibrils upon the mechanical training. This adaptive capability is highly expected in artificial materials, particularly in hydrogel actuator. In order to avoid the failure for devices by suffering from the accumulated mechanical loading, in this work, a double layered thermo‐responsive hydrogel actuator capable of self‐strengthening was successfully prepared. In the bilayer, PVA nanocrystals with different particle sizes were uniformly distributed in each monolayer matrix, giving rise to the asymmetric structure and the resultant differentiated de‐swelling behaviors. Thus, the obtained hydrogel actuator with the semi‐interpenetrating network of P(NIPAM‐co‐NMA) can display diverse programmable transformations by varying the temperatures. The existence of PVA nanocrystals in both layers not only can enhance the mechanical strength, dramatically minimizing the collapse of hydrogel actuator in service due to the imbalance of the mechanical properties for bilayer structure, but also was greatly involved in the self‐reinforcing behavior. After repetitive tensile training with 80% strain, the tensile strength and fracture strain increased from 29.6 to 45.8 kPa and 95% to 104%, respectively. The experimental results indicated that the anisotropic orientation and strain‐induced‐crystallization for PVA crystalline domains readily occurred along the tensile direction, finally leading to the synchronous enhancement in mechanical strength for both layers. This work provides a new strategy for designing smart and robust biomimetic hydrogel systems that can be further used as the intelligent soft robotics in various fields.