The mechanical performance of superelastic NiTi with various grain sizes (GSs) in nanocrystalline regime (GS < 30 nm) are investigated. With the help of digital image correlation, both global and local mechanical responses of NiTi during quasi-static test and fatigue cycling are recorded. If GS is below 14 nm, NiTi deforms homogenously; if GS is above 14 nm, NiTi deforms in a heterogeneous manner. The mechanical response, the fatigue life, the dissipation energy and the resistance to the dissipation energy degradation of nanostructured NiTi are addressed and analyzed. The results indicate that the mechanical performance of NiTi can be designed and optimized by controlling GS in a moderate regime.