In this study, an innovative process, electrically assisted ultrasonic nanocrystal surface modification (EA‐UNSM), is used to process Ti6Al4V alloy. As compared with traditional UNSM, EA‐UNSM results in lower dislocation density and larger grains due to the thermal annealing effect caused by resistive heating. In addition, deeper plastic deformation layer is observed in the electrically assisted case. By supplying mechanical energy and thermal energy simultaneously, a strong dynamic precipitation effect is induced, which generates nanoscale precipitates in the EA‐UNSM‐treated Ti6Al4V alloy. These nanoscale precipitates can effectively pin dislocations during plastic deformation and thus significantly improve the surface hardness.