A nanocrystalline (NC) layer with the thickness of 30 μm was produced on pure titanium surface by surface mechanical attrition treatment (SMAT). Microstructure observation indicated that the grain size increases with depth from the treated surface. The friction coefficient decreases and the wear resistance increases with the SMAT sample as compared to its coarse-grained counterpart. The improvement of the wear properties could be attributed to the higher hardness of SMAT sample.