In hardening stage, a model was used to study the plastic deformation behaviors of nanocrystalline materials. The material was considered as a composite of grain interior phase and grain boundary (GB) phase. The constitutive equations of the two phases were determined in term of their main deformation mechanisms. In softening stage, a shear band deformation mechanism and the corresponding constitutive relation were presented. Calculation results have shown that the predications fit well with experimental data. The investigation using the ﬁnite-element method (FEM) provided a direct insight into quantifying shear localization effect in nanocrystalline materials.