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The efficacy of peening treatment depends on the plasticity of the target metal. In this study, the effectiveness of high-amplitude short duration pulsed current in improving the peening efficacy was examined in a process called electropulsing-assisted ultrasonic nanocrystal surface modification (EP-UNSM). During the EP-UNSM process, the target metal, i.e., Ti64, is subjected to simultaneous ultrasonic peening and electropulsing. The high energy pulsed current can generate a critical magnetic field that can induce the transition of the radical pairs formed by dislocations and the pinning obstacles from the singlet state to the triplet state. This leads to higher dislocation mobility and thus higher plasticity for more effective peening treatment. The results show that the sample treated with EP-UNSM had a deeper plastically deformed layer than that for samples subjected to UNSM and continuous current–assisted UNSM (CC-UNSM), and the maximum depth of plastic deformation was obtained when using the highest peak current density. Due to microstructure refinement, work hardening, and dynamic strain aging, the EP-UNSM sample had a 50% higher surface hardness compared with the control sample. Moreover, the compressive residual stresses generated by EP-UNSM were higher in magnitude and greater in depth compared to those generated by traditional UNSM. These results demonstrate that pulsed current can effectively improve the peening efficacy and EP-UNSM is an effective method for strengthening Ti64. • Pulsed current leads to higher dislocation mobility and thus higher plasticity for more effective peening treatment. • EP-UNSM generates a gradient nanocrystalline layer in Ti64. • EP-USM results in high surface hardness and higher residual stress magnitude and depth. [ABSTRACT FROM AUTHOR]