Robust yet Self-Healing Multimodal Actuators Enabled by Noncovalent Assembled Nanostructure

In nature, animals can realize multimodal movements such as walking, climbing, and jumping through transformation in locomotor gaits or form for survival, which is highly desired for untethered flexible actuators yet remains challenging. Here, we propose a robust self-healing multimodal actuator enabled by noncovalent assembled nanostructures with elaborate regulation of multistage responsive behaviors. Owing to the dynamic interfacial design between multiple components, the stimulus can be accurately delivered through a "light-heat-force release" pathway, endowing the actuator with diverse motion capabilities and desired jumping ability (27 cm, 34 times body length). Moreover, the reversible recombination and sliding properties of the noncovalent assembled dynamic network ensure high toughness (81.9 kJ/mol) and self-healing efficiency (88.2%), which greatly benefit the long-term service under complex and demanding scenarios. This study provides a strategy for the design of multimodal flexible actuators to improve their adaptability and stability in complex environments.