Ultra‐Stretchable, Variable Modulus, Shape Memory Multi‐Purpose Low Hysteresis Hydrogel Derived from Solvent‐Induced Dynamic Micelle Sea‐Island Structure

Abstract The rapid development of sensors and soft robotics has substantially increased the demand for unique hydrogels with diverse high performance. However, it remains a challenge to prepare a multi‐purpose hydrogel via a facile approach. By virtue of copolymerization of acrylamide (AM) and acryloyl Pluronic 127 (PF127‐DA), a novel type of ultra‐stretchable (435–2716%, 10–40 wt%), variable modulus (0.36–112.79 MPa, 30 wt%), tough (1.13–7.17 MJ m −3 , 10–40 wt%), low hysteresis (about 10%, 30 wt%), transparent (27.98–83.78%, 10–40 wt%), and shape memory (fixation ratio up to 97%, recovery ratio up to 100%, 10 wt%) hydrogels derived from dynamic micelle sea‐island structure are prepared. The new strategy of using solvent‐induced crystallization of the polyethylene oxide segments of PF127‐DA molecular chain and matrix volume phase transition to achieve variable modulus and shape memory is a purely physical process that can be performed cyclically. Notably, this design reflects the important role of PF127‐DA micelles in optimizing mechanical properties and intelligence. Additionally, PAM/PF127 hydrogels display a high sensitivity toward deformability, elasticity, solvent‐induced shape memory, and variable modulus properties by which it can be used for stress sensors, damping pads, and mechanical bearing. These novel types of hydrogels could be applicable into multifunctional and adaptive platforms.