Using the impact test and finite element simulation, the failure behavior of the Mo-modified layer on pure Ti was investigated. In the impact test, four loads of 100, 300, 500, and 700 N and 10 4 impacts were adopted. The three-dimensional residual impact dents were examined using an optical microscope (OlympusDSX500i), indicating that the impact resistance of the Ti surface was improved. Two failure modes cohesive and wearing were elucidated by electron backscatter diffraction and energy-dispersive spectrometer performed in a field-emission scanning electron microscope. Through finite element forward analysis performed at a typical impact load of 300 N, stress-strain distributions in the Mo-modified Ti were quantitatively determined. In addition, the failure behavior of the Mo-modified layer was determined and an ideal failure model was proposed for high-load impact, based on the experimental and finite element forward analysis results.