Abstract The photo‐responsive intelligent actuators with noninvasiveness, remote controllability, convenient energy transmission, and rich light sources, have become one of the most concerned drives. However, the complex preparation processes, high costs, poor convenience, complex structures, and low sensitivity, restricting their further application. In this work, we propose a double‐layer flexible photo‐driven composite film of graphene oxide‐carbon nanotube‐polydimethylsiloxane/polyethylene (GO‐CNT‐PDMS/PE), which has achieved the efficient conversion of GO‐CNT‐PDMS/PE photo‐driven films from photo energy to thermal energy and then to mechanical energy. The COMSOL finite element simulation model is established and simulated. A two‐stage conversion model of “photo‐heat‐mechanical energy” is proposed to verify the thermal response of the material and the photo‐driven mechanism. The influence of different thicknesses of photothermal layers (GO‐CNT‐PDMS) and GO‐CNT concentrations on the performance of double‐layer flexible optical drivers are studied. Based on the optimized GO‐CNT‐PDMS/PE flexible photo‐driven composite film, the designed near‐infrared photo‐driven flexible soft robots grippers have achieved photo‐controlled bending deformation and successfully grasped the target object. The feasibility of it in micro‐nano operation scenarios is verified by adjusting the light intensity and duration, controlling the opening and closing angle of the gripper and the grasping force. This research is expected to promote the technological development in fields such as intelligent equipment, precision medicine, and environmental monitoring.