Photoresponsive soft actuators with the unique merits of flexibility, contactless operation, and remote control have huge potential in technological applications of bionic robotics and biomedical devices. Herein, a facile strategy was proposed to prepare an intrinsically-photoresponsive elastomer by chemically grafting carbon nanotubes (CNTs) into a thermally-sensitive liquid-crystalline elastomer (LCE) network. Highly effective dispersion and nematic orientation of CNTs in the intrinsic LCE matrix were observed to yield anchoring energies ranging from 1.65 × 10-5 J m-2 to 5.49 × 10-7 J m-2, which significantly enhanced the mechanical and photothermal properties of the photoresponsive elastomer. When embedding an ultralow loading of CNTs (0.1 wt%), the tensile strength of the LCE increased by 420% to 13.89 MPa (||) and 530% to 3.94 MPa (⊥) and exhibited a stable response to repeated alternating cooling and heating cycles, as well as repeated UV and infrared irradiation. Furthermore, the shape transformation, locomotion, and photo-actuation capabilities allow the CNT/LCE actuator to be applied in high-definition biomechanical applications, such as phototactic flowers, serpentine robots and artificial muscles. This design strategy may provide a promising method to manufacture high-precision, remote-control smart devices.