Hierarchically Structured Self‐Healing Actuators with Superfast Light‐ and Magnetic‐Response

Despite the tremendous advancement of intelligent robots, it remains a great challenge to integrate living organisms‐like multistimuli responsive actuation and excellent self‐healing ability into one single material system, which will greatly benefit and broaden the development of smart biomimetic materials. Herein, a novel self‐healable multistimuli responsive actuator is developed based on hierarchical structural design and interfacial supramolecular crosslinking. The resulting biomimetic actuator shows a record high photothermal efficiency (η PT = 79.1%) and thermal conductivity (31.92 W m −1 K −1 ), and presents a superfast actuating response (near‐infrared light: 0.44 s; magnetic field: 0.36 s). In addition, the supramolecular crosslinking endows excellent self‐healing performance in both mechanical and actuating properties to the material. This biomimetic actuator with its hierarchical structure design provides great potential for various applications, such as artificial muscles, soft robotics, and biomedical microdevices.