Liquid crystal elastomers (LCEs) blended with photothermal nanofillers can reversibly and rapidly deform their shapes under external optical stimuli. However, nanointerfacial slipping inevitably occurs between the LCE molecules and the nanofillers due to their weak physical interactions, eventually resulting in cyclic instability. This work presents a versatile strategy to fabricate nanointerfacial-slipping-restricted photoactuation elastomers by chemically bonding the nanofillers into a thermally actuatable liquid crystal network. We experimentally and theoretically investigated three types of metal-based nanofillers, including zero-dimensional (0D) nanoparticles, one-dimensional (1D) nanowires, and two-dimensional (2D) nanosheets. The toughly crosslinked nanointerface allows for remarkably promoted interfacial thermal conductivity and stress transfer. Therefore, the resultant actuators enable the realization of long-term-cyclic-stability 4D-printed flexible intelligent systems such as the optical gripper, crawling robot, light-powered self-sustained windmill, butterflies with fluttering wings, and intelligent solar energy collection system.