In this study, the mechanical properties of Cu-Zr binary bulk metallic glasses (BMG) were investigated at the nano-scale. The stable amorphous structures and corresponding energies of BMG structures are performed by density functional theory (DFT) calculation as reference data. This study will combine the Force-Matching (FM) method and Basin-Hopping (BH) method to develop a new method for fitting the Cu-Zr Tight-binding (TB) potential parameters. Moreover, the Bulk modulus, Shear modulus, Young's modulus and Poisson ratio of Cu46Zr54, Cu50Zr50 and Cu64Zr36 structures are calculated with the fitting TB parameters. In addition, the compression process of BMG materials is simulated by the Molecular Statics. The stress and strain are obtained to investigate the deformation mechanism of CuZr/Zr/CuZr nanolaminates at 0 and 45 inclined degree. Finally, we investigate the angle in the deformation process under different strain in the shear band, shear transformation zones (STZs) and force caused by the slip of the atomic distribution of TFMGs layer.