Heterogeneous gradient nanostructures induced through surface treatment of nickel-based superalloys hold significant promise for enhancing wear resistance. In this study, a 700 µm ultra-thick gradient nanostructured (GNS) strengthening layer was fabricated on the surface of an Inconel 625 alloy plate via surface mechanical rolling treatment (SMRT). Subsequently, the tribological behaviors and wear resistance mechanisms of coarse-grained (CG) and GNS samples at temperatures ranging from 25 ℃ to 800 ℃ were comparatively investigated. The results indicated that the gradient nanostructures significantly enhanced the high-temperature wear resistance of the samples, which wear characterized by low coefficient of friction (COF), wear rate and thin friction layer. This enhancement was attributable to the stability and excellent hot hardness of the gradient nanostructures during friction.