When NIR light is applied, the strips convert heat into kinetic energy, and segments closer to the center exhibit more pronounced contraction due to variations in surface stress. All segments autonomously return to the flat state when the light is off, in a reversible and repeatable manner. Controlled directional locomotion is achieved by manipulating the incidence direction and cycles of NIR light. The four-fingerlike robot serves as the foundation for a soft gripper. The fingers coated with TMC/CNF bend inward upon stimulation, and this bending behavior can be converted into gripping force. As illustrated in Figure , the soft gripper is designed to delicately grasp and manipulate objects. It demonstrates practical application by lifting and moving a piece of foam weighing 4.5 times its own weight, highlighting the impressive strengthto-weight ratio of these actuators. Notably, our plasma-ALE-treated TMC/CNF soft robotics exhibit a fast response time (~4.23 s) and an ultra-large bending angle (165°), outperforming other 2D material-based actuators without plasma-ALE treatment. This capability is particularly beneficial for applications in biomimetic robotics and biomedical devices like artificial muscles. These results demonstrate that plasma-ALE-treated TMC/CNF actuators enable the fabrication of intricate and multifunctional structures in soft robotics.