By performing severe plastic deformation treatment, surface gradient nanocrystalline structure can be obtained on the surface of 06Cr19Ni10 and consequently, its cavitation resistance can be imporved. In this research, the high-energy shot peening method was used. Gradient nanocrystalline structures with different tissue structures were obtained by adjusting the shot peening pressure within the range of 0.3~0.6 MPa. Optical microscope, X-ray diffractometer and microhardness tester were used to perform morphology, phase analysis and cross-section hardness analysis on the gradient nanocrystalline structures. In addition, electrochemical workstation and self-made cavitation tester were used to examine the corrosion resistance and cavitation resistance of gradient nanocrystalline structures. Results of the cross-section metallography showed that by adjusting the shot peening pressure, a layer of gradient nanocrystalline structure with thickness of 50~100 μm can be formed on the surface of 06Cr19Ni10; XRD results showed that shot peening can broaden (111), (200), (220), (311), (222) diffraction peaks of the crystal orientation. According to the calculation using Voigt function method, the grain size of the top layer of the gradient nanocrystalline structure was in the range of 32~87 nm and the surface hardness was increased from 180HV0.05 to 360~525HV0.05. In addition, shot peening can increase the self-corrosion potential of 06Cr19Ni10 to ?0.385 V (vs. SCE) and reduce its self-corrosion current density to 3.512 μA/cm2, thus, significantly extend its cavitation incubation period. The maximum cavitation corrosion resistance coefficient is approximately 12.92 times of that of the untreated sample. The gradient nanocrystalline structure can comprehensively improve the surface characteristics of 06Cr19Ni10, and ultimately improve its cavitation resistance performance.