In this study, a batch of indium tin oxide (ITO)/Sn composites with different ratios was obtained based on the principle of thermal evaporation by an electron beam. The crystalline structure, surface shape, and optical characterization of the films were researched using an X-ray diffractometer, an atomic force microscope, a UV-Vis-NIR dual-beam spectrophotometer, and an open-hole Z-scan system. By varying the relative thickness ratio of the ITO/Sn bilayer film, tunable nonlinear optical properties were achieved. The nonlinear saturation absorption coefficient β maximum of the ITO/Sn composites is -10.5×10-7cm/W, approximately 21 and 1.72 times more enhanced compared to monolayer ITO and Sn, respectively. Moreover, the improvement of the sample nonlinear performance was verified using finite-difference in temporal domain simulations.