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.