In this paper, we report on the microstructural evolution and mechanical properties of a 5052 Al alloy processed by rotationally accelerated shot peening (RASP). A thick deformation layer of ∼2 mm was formed after the RASP process. Nano-sized grains, equiaxed subgrains, and elongated subgrains were observed along the depth of the deformation layer. Dislocation accumulation and dynamic recrystallization were found primarily responsible for the grain refinement process. An obvious microhardness gradient was observed for all of the samples with different RASP processing parameters, and the microhardness in the top surface of 50 m/s-5 min RASP-processed sample is twice that of its coarse-grained (CG) counterpart. The yield strengths of the RASP-processed 5052 Al alloy samples were 1.4–2.6 times that of CG counterparts, while retaining a decent ductility (25–84% that of CG). The superior properties imparted by the gradient structure are expected to expand the application of the 5052 Al alloy as a structural material.