Realization of surface-reinforced aluminum alloys with excellent corrosion resistance remains a major topic. Herein, a novel method based on combination of electron beam evaporation plating and surface alloying was proposed. Results revealed that the current density is one order of magnitude less than that of the substrate and that the impedance value is doubled. The nanometer-scale refinement of the grains and the homogenous dispersion of nanocrystallization Al2Cu in the modified layer of aluminum alloy contributed to the enhancement of corrosion resistance. This study is expected to provide a new sight for the development of Cu-reinforced high-performance aluminum alloys.