NiTi shape memory alloy was processed by femtosecond laser shock peening (FLSP) without protective coating in distilled water to modify its surface characterizations. The surface topography, microhardness, microstructure and scratch testing were studied before and after FLSP treatment. The experimental results show that FLSP with different laser scanning speeds and passes can change the surface roughness and microhardness due to laser ablation and high pressure of shock wave. The average microhardness value of the specimens FLSPed in distilled water increased. Grain refinement was observed in the surface layer of FLSPed NiTi alloy. The scratch testing revealed that FLSP process can decrease the frictional force and coefficient of friction, and it also demonstrated that the FLSP technique is beneficial to enhance the surface wear property of NiTi alloy.