The precise manipulation of grain boundary microstructure, including interfacial solute partition and precipitate distribution, is crucial for regulating the corrosion resistance of age-hardening aluminum alloys. In this study, we explored a novel manipulation pathway, the pulsed electric field (PEC), to regulate solute segregation to grain boundary to form a specific grain boundary structure. The calculated atomic diffusion results reveal that the PEC can stimulate atomic diffusion by decreasing the energy required for diffusion, through which the continuous distribution of grain boundary precipitates and solute depletion zone formation can be inhibited. Hence, the corrosion resistance is significantly improved.