Abstract Ti 3 C 2 T x MXene film is promising for low‐voltage electrochemical actuators due to its excellent electrical conductivity, volumetric capacitance, and mechanical properties. However, its in‐plane actuation is limited to little intralayer strain of MXene sheets under polarization. Here we demonstrate that a simple tetrabutylammonium (TBA) functionalization of MXene improves the in‐plane actuation strain by 337% and also enhances the mechanical property and stability in air and the electrolyte. Various in situ characterizations reveal that the improved actuation is ascribed to the co‐insertion/desertion of TBA and Li ions into/from MXene interlayer galleries and inter‐edge gaps that causes a large in‐plane sliding of MXene sheets under negative/positive polarizations. The assembled bending actuator has a high strength and modulus and generates a peak‐to‐peak strain difference of 0.771% and a blocking force up to 51.5 times its own weight under 1 V. The designed soft robotic tweezer can grasp an object under 1 V and hold it firmly under 0 V. The novel sheet sliding mechanism resembling the filament sliding theory in skeletal muscles may inspire the design of high‐performance actuators with other nanomaterials. This article is protected by copyright. All rights reserved