The effects of electropulsing-assisted ultrasonic surface rolling process on surface mechanical properties and microstructure evolution of commercial pure titanium were investigated. It was found that the surface mechanical properties were significantly enhanced compared to traditional ultrasonic surface rolling process (USRP), leading to smaller surface roughness and smoother morphology with fewer cracks and defects. Moreover, surface strengthened layer was remarkably enhanced with deeper severe plastic deformation layer and higher surface hardness. Remarkable enhancements of surface mechanical properties may be related to the gradient refined microstructure, the enhanced severe plastic deformation layer and the accelerated formation of sub-boundaries and twins induced by coupling effects of USRP and electropulsing. The primary intrinsic reasons for these improvements may be attributed to the thermal and athermal effects caused by electropulsing treatment, which would accelerate dislocation mobility and atom diffusion.