Photoreversible Polyurea Actuators With Spatiotemporal Control and Adaptive Mechanics

Biological systems can adapt to dynamic environments through the modulation of their local stiffness and reorganization of internal structures. Achieving comparable multifunctional adaptability in synthetic materials—especially within wireless, miniaturized, and programmable platforms—remains a considerable challenge. Herein, we report a light‐ and temperature‐responsive actuator system based on a dynamic polyurea network incorporating anthracene units capable of reversible [4 + 4] photodimerization. This dual‐mode molecular design allows spatiotemporal modulation of network connectivity and mechanical properties, enabling nearly 400‐fold modulation of Young's modulus. The actuator features programmable anisotropy, self‐healing, photopatterning, and photowelding properties, enabling adaptive gripping behaviors akin to an elephant trunk, including reversible 3D morphing, load‐bearing actuation, and mechanical logic encoding. This work proposes a molecularly tunable, photoreversible platform for reconfigurable actuation, offering new opportunities in soft robotics, information storage, and adaptive mechanical systems.