In this study a CAE-assisted nano-indentation measurement system has been development and applied for quantitatively evaluating the elastic properties of anisotropic thin films. The measurement system is based on a nano-indentation test with a spherical indenter and the optimal process was simulated with the FEM. A thin Al film was sputtered onto a Si substrate and used as the test-piece. The anisotropic mechanical properties of the thin films were measured by the proposed CAE-assisted nano-indentation measurement system. For evaluation of the anisotropy, the orientation of the crystallines of the thin film was measured by X-ray diffraction, and the cross-section of the thin film was observed by a TEM. The results show that the thin film has anisotropic characteristics, and that the proposed CAE-assisted nano-indentation measurement system provides the anisotropic mechanical properties appropriately.