Titanium alloys are widely used in industry because of their excellent mechanical properties, but their applications are limited due to their poor wear resistance. In this study, we attempted to improve the surface hardness of titanium alloys by applying an atomic rearrangement technique using high-frequency current application. Vickers hardness tests were conducted after the application of high-frequency current, and the surface Vickers hardness was improved by 8.2% at the maximum. Dislocation density was measured using an X-ray diffraction method to evaluate the microstructural change, and an increase in the dislocation density of the α-phase was confirmed. These results suggest that high-frequency current treatment is effective in improving the wear resistance of titanium alloys.