The structural vulnerability and immobility of the multi‐responsive actuators restrict its application in soft robots. Hence, self‐healing film actuators based on interfacial supramolecular crosslinking and hierarchical structural design have been developed. The graphene oxide supramolecular film with asymmetric structure reveals excellent reversible deformation under different trigger signals like moisture, thermal, and infrared light. Meanwhile, it shows a good healing property based on supramolecular interaction, achieving the structure restoration and reconstitution of stimuli‐responsive actuators (SRA). The re‐edited SRA realizes reverse reversible deformation under the same external stimuli. To enhance the functionality of graphene oxide‐based SRA, the reconfigurable liquid metal could be modified on the surface of the graphene oxide supramolecular film at low temperature (defined as LM‐GO) due to its compatibility for hydroxyl. The fabricated LM‐GO film displays satisfactory healing property and good conductivity. Besides, the self‐healing film maintains strong mechanical strength, which can bear more than 20 grams of weight. This study provides a novel strategy to fabricate self‐healing actuator with multiple responses, accomplishing the functional integration of the SRAs.
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