•OH), replacing original surface termination atoms with OH/O -groups to form an O-dominated surface. Conversely, Ar plasma treatment causes physical etching through strong ion bombardment to remove surface terminations. Literature also indicates that adding Ar gas to O 2 plasma increases the density of high-energy electrons and provides more active sites for O-containing functional groups, enhancing the replacing efficiency of O 2 plasma. CNFs were added into TMC to form the TMC/CNF actuation material system. TMC/CNF composites are widely explored due to their synergistic properties. The integration of CNFs into TMC-based materials significantly improves structural integrity, water retention, and thermal management of TMC, making them ideal for applications in soft robotics, flexible electronics, and adaptive devices. Several studies have demonstrated the effectiveness of TMC/CNF composites in enhancing actuator performance, particularly in response to external stimuli like near-infrared (NIR) light. In this study, we developed a plasma-enabled atomic layer etching (plasma-ALE) technique to engineer the surface terminations of Ti 3 C 2 Tₓ (hereinafter referred to as TMC). ALE is a top-down method enabling atomic-level modification of TMC surface chemistry. Through O 2 /Ar plasma ALE, most of the surface terminations of TMC were tailored into -OH and =O, resulting in an 80% increase in electrical conductivity and enhanced photothermal conversion efficiency. Furthermore, we fabricated a bimorph actuator by depositing TMC/cellulose composites onto a polycarbonate (PC) membrane using vacuum filtration. After plasma-ALE treatment, TMC/cellulose soft robotics exhibits a 29% increase in bending angle and a 21% enhancement in bending force under near-infrared (NIR) light. This study also validates the compatibility of plasma-ALE treatment with various manufacturing methods and soft robotics systems, with efficacy across multiple scales ranging from millimeter to centimeters.