The Al/Cr double-layer film structure samples (thickness, 1200 nm) were prepared by the magnetron sputtering method. To investigate the mechanical properties, the samples were measured by using a nanoindentation instrument. The test results showed the nonlinearity and different modes of the main mechanical properties by comparing the macro-scale structure samples with other samples of similar materials. Based on the test, the elastic modulus and hardness of thin film structures can be calculated by considering different loads to conduct multi-point indentations. Meanwhile, the relationships between the mechanical parameters can be investigated based on these Al/Cr double-layer film structure samples. To validate the test, numerical analysis was developed using a finite element method to simulate the loading and unloading process of indentation. The simulation results were compared with the results of experiments to illustrate the validity of both the test and simulation to a certain extent. The investigation builds not only an experimental basis for practical applications for future study, but also supplies a complementary means of verification for theoretical analysis. (C) Koninklijke Brill NV, Leiden, 2011