MXene nanosheets are promising to be ultrathin solid lubricant or interface solving the friction and wear problems of miniaturized equipment. Here, the frictional behaviors and adhesive properties of the Ti₃C₂, F-Ti₃C₂, and TMA-Ti₃C₂ nanosheets were explored by atomic force microscope for the first time. The nanofrictional behavior of TMA-Ti₃C₂ was significantly different from that of Ti₃C₂ and F-Ti₃C₂. The friction of TMA-Ti₃C₂ increased slightly and then decreased as the load decreased, leading to the appearance of a negative friction factor; the frictions of Ti₃C₂ and F-Ti₃C₂ decreased with decreasing load, resulting in positive friction factors. Meanwhile, because the surface of TMA-Ti₃C₂ was more hydrophilic than that of Ti₃C₂ and F-Ti₃C₂, the friction and adhesion of TMA-Ti₃C₂ were greater than those of Ti₃C₂ and F-Ti₃C₂. It indicated that the surface properties played an important role in the adhesion and friction. Hence, adjusting the surface properties of MXene nanosheets will provide a new direction for designing solid lubricants and nanointerfaces in micro- and nanoelectromechanical systems.