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The hybrid films bent reversibly upon alternate irradiation with ultraviolet and visible light. The hybrid films bent as fast as single crystals, even when larger than single-crystal size, showing great mechanical performance originating from the advantages of both molecular crystals (fast response time) and polymers (large size). This work enriches the development of light-driven hybrid actuators composed of molecular crystals and polymers.Space manipulators have attracted much attention due to their implications in on-orbit servicing in