Laser shock peening, an advanced technology for severe surface plasticity peening, encounters challenges such as shallow hardened layers and surface spalling when dealing with difficult-to-machine materials. In this study, we introduced a high-frequency electropulsing-assisted laser shock peening (HFEP-LSP) technique that coupled laser shock peening with high-frequency electric pulses to achieve a significant and deeper plastic deformation layer. In the HFEP-LSP technique, we first considered the dual “skin effect”, which coupled the skin effect of high-frequency electric pulses with the “skin effect” of the mechanical effect induced by the laser shock wave. An integrated experimental platform comprising an electric pulse generator, laser shock peening equipment, and a control system was built. A >1.6 mm deep compressive residual stress layer was obtained, and the depth of the plastic deformation layer increased by 83.3 %. Furthermore, we elucidated the dual “skin effect”-induced complex heterostructure and βm phase transition. A comprehensive analysis revealed the factors contributing to the deeper strengthening layer induced by HFEP-LSP, including the compressive residual stress and plastic deformation layers. In addition, the effects of laser shock peening and HFEP-LSP on the mechanical properties were investigated. Compared to the annealed samples, the ultimate tensile strength and elongation of the HFEP-LSP-treated samples were increased by 12.3 % and 57.1 %, respectively, with a fatigue life improvement of 176.4 %. The mechanism of synergistic improvement in strength and ductility was demonstrated.