Introducing nanotwins into materials is one of the important strengthening methods to achieve the synergistic improvement of strength and ductility. The anisotropic mechanical behaviors of nanotwinned materials have been widely studied by experimental and computational methods. The dominant deformation mechanisms about dislocation slippages can be effectively switched among three modes, and controlled by twin spacing and the angle between twin boundaries (TBs) orientation and loading direction. Particularly, most of previous researches mainly focused on the deformation mechanisms during the plastic flow stage and researchers paid little attention on the anisotropic characteristics of TBs at the elastic stage which are also essential to manufacture the high-performance materials. Therefore, this study is aiming to systematically investigate the anisotropic effect of TBs both at the elastic and plastic stages within the single crystalline or polycrystalline systems by molecular dynamics (MD) simulations. It is revealed that, when the loading direction is parallel to twin planes, the introduction of TBs in single crystalline models will significantly affect the characteristics of atomic bond rotation and elongation dominated elastic deformation, which can alter the Poisson’s ratio of materials, generate elastic-softening behavior and inhomogeneous elastic deformation. At the plastic flow stage, the deformation mechanism transforms from trans-twin dislocation slippage into the coexistence of Hard Mode I and threading dislocation slippage (Hard Mode II) when the loading direction changes from parallel to perpendicular direction with respect to TBs. Moreover, the dislocation segments at the conjunction of trans-twin dislocation play a momentous role in enhancing material strength. The results for polycrystalline models are consistent with that of single crystalline ones. These findings are expected to be beneficial for the development of high-performance nanostructured materials for structural and functional applications by strain engineering and defect regulation.