Immiscible Cu-Fe alloys exhibit poor corrosion resistance due to different corrosion potentials between the constituent phases, which limits their application. In this paper, a composite gradient-structured Cu-10 wt.%Fe plate was prepared via the ultrasonic surface rolling process (USRP). The microstructure evolution, mechanical properties and corrosion behavior were studied. The results demonstrate that USRP effectively enhances both the strength and corrosion resistance of the Cu-10Fe alloy. The improved strength is related to the combined effects of Hall–Petch strengthening, dislocation strengthening, and additional strengthening resulting from homogeneous deformation between the surface layer and the matrix. The enhanced corrosion resistance is primarily attributed to the refined microstructure of the surface layer after USRP, which facilitates the formation of a protective passivation film.