Gradient nanostructure in aluminum alloy, constructed via a two-dimensional ultrasonic surface burnishing process, displays enhanced tribocorrosion resistance in artificial seawater. Corrosion tests are undertaken to understand the influence of gradient nanostructure on corrosion resistance, and crystal plasticity finite element models are developed to examine wear resistance. Tribocorrosion tests are performed through wear tests in the artificial seawater environment. The results indicate that the processed samples' corrosion rate decreases from 3.12 × 10−2 mm/a to 2.45 × 10−3 mm/a. The wear scar sizes of the processed samples are approximately half the unprocessed samples. The gradient nanostructure obstructs dislocation glide during wear, diminishes the accumulation shear, and promotes high-hardness corrosion product formation, effectively isolating the direct contact between the friction pairs, thus improving the tribocorrosion resistance.