Perfluoropolyether (PFPE) lubricant is widely used in plenty of cutting-edge technologies because of its extraordinary properties. However, poor boundary lubrication and creep limit their further applications. Here, we demonstrated a PFPE supramolecular gel with surface-functionalized Ti3C2Tx as additives for highly efficient boundary lubrication and prevention of creep. It turned into an oily liquid at 124.5 °C, accompanied by a rapid decrease in viscosity. Additionally, the phase transition could be achieved by shear stress. This kind of gel reduced wear volume by 90.75% compared with pure PFPE oil. Its friction coefficient (∼0.113) varied slightly with time. Notably, its load-bearing capacity exceeded 1500 N. This work puts forward an approach to the preparation of PFPE-based supramolecular gel lubricant with surface-functionalized Ti3C2Tx additive.