The 6061 aluminum alloys are treated by laser shock peening (LSP), and the effects of LSP on their wear resistance and electrochemical properties are investigated. The micro-hardness, residual stress, and so on are examined and analyzed. The results show that, LSP can effectively enhance the mechanical properties of samples. On the surfaces of the LSP treated specimens, there is no phase change, but the micro-hardness and residual stress increase obviously, and the corrosion resistance of 6061 aluminum alloys is obviously improved. The friction coefficients before and after the LSP treatment are comparable, but the wear loss of the LSP treated specimen decreases and the wear resistance is significantly improved.