“…Polymer-based shape change materials or actuators have advantages, such as lightweight, high flexibility, and low cost, with tremendous application prospects in artificial muscles, [1,2] soft DOI: 10.1002/adfm.202308677 robots, [3,4] electrical control, [5] environmental exploration [6] and intelligent sensors [7,8] and wearables. [9,10] To this end, several categories of functional polymers and polymer-based composites have been developed in terms of molecular design [11,12] and microstructural regulation, [13] including: 1) shape memory polymers [14,15] and liquid crystal elastomers [16][17][18] based on interactions and alignment-isotropy transition of molecular chains, 2) dielectric elastomers [19,20] or ionic polymermetal composites (IPMCs) [21] based on electrostatic repulsion/solvated ions migration, 3) composites with multilayer or gradient structures [22][23][24][25][26] relying on the differences in thermal expansion coefficients or swelling behaviors, and 4) phase change material (PCMs) filled polymer-based composites relying on volume expansion/contraction, [27,28] regulation of crystallization behavior and mechanical properties [15] or segmental fixation/release effect [13,29,30] of solid-liquid phase transition process. However, most of the above strategies rely on light-or heatdriven modes and produce unsatisfactory performance.…”