Cryomilled Cu-Al powder and the Cu/Al mixture were sprayed onto aluminum substrate using the cold spraying process. This study focused on the wear properties of the nanocrystalline (NC) Cu-Al coating in comparison to its coarse-grained (CG) Cu/Al counterpart. The results showed that the as-sprayed deposit presented a dense microstructure. Investigations on the worn surface of the NC coating revealed that the plastic deformation with grooves and some debris were prominent with no visible cracking. Nanocrystalline Cu-Al coating showed a good wear resistance with a low friction coefficient. The enhancement of the wear properties of the NC Cu-Al was attributed to the grain refinement and the superior hardness.