High-entropy alloys (HEAs) have attracted much attention due to their excellent mechanical properties. Due to their typical entropy effect, sluggish diffusion, and cocktail effect, HEAs show unexpected performance and have a good prospect in the industry. [1][2][3][4][5] The mechanical properties of HEAs are closely related to the microstructure of materials. Therefore, many researchers have studied the relationship between the microstructure and mechanical properties of HEAs. For example, Nikitin reported that the mechanical properties of CrMnFeCoNi at low temperatures were better than those at room temperature. [6] This is because the deformation mechanism at room temperature mainly involves plane slip dislocation activity, while that at low temperature mainly involves nanotwinning. It was also found by the molecular dynamics (MD) study where dislocation slip replaces grain boundary slip to control plastic deformation of Co 25 Ni 25 Fe 25 Al 7.5 Cu 17.5 at low temperature and high strain rate. [7] Picak demonstrated that Fe 40 Mn 40 Co 10 Cr 10 has different plastic deformation modes in different orientations, and the formation of nanotwins and high-density dislocations enabled the HEA to have high strength without sacrificing ductility. [8] Gubicza showed that the grain refinement and high-density dislocations could significantly improve the strength and ductility of HEA, and the contribution of grain refinement was greater than that of high-density dislocation. [9] In addition, the beneficial microstructure in materials could be induced by severe plastic deformation. [10,11] So, regulating the microstructure of materials through plastic deformation is an effective way to improve the mechanical properties of HEAs.As a widely used surface treatment method, laser shock peening (LSP) can generate strong shock waves inside the workpiece to induce the plastic deformation of the material, resulting in favorable residual stress and beneficial microstructures such as high-density dislocations in the workpiece. [12][13][14] Therefore, many studies have obtained high-strength alloys using LSP to control the microstructure of the materials. [15][16][17] For example, high strength and ductility in selective laser melting (SLM) Ti-6Al-4 V alloy were obtained using the LSP process. [18] After LSP treatment, the yield strength and fatigue life of friction stir-welded CuCrZr sheets were increased by about 35% and 70%