The effects of ultrasonic nanocrystal surface modification (UNSM) treatments on the microstructure, mechanical, and corrosion behavior of LZ91 Magnesium–Lithium (Mg–Li) alloy were systematically investigated. The results show that UNSM treatments have greatly positive effects on the mechanical and corrosion behavior improvements. As compared to the bare sample (BS), the near-surface grains were refined and the surface roughness (R_a) of the sample was reduced from 0.514 µm to 0.082 µm; and the maximum hardness and tensile yield strength remarkable increased by 70% and 65.4% after UNSM treatments, respectively. In addition, the corrosion behavior of LZ91 Mg–Li alloy was also improved after UNSM treatments. The mechanical and corrosion behavior improvements can be attributed to the introduced thick hardening layer with low roughness and smaller grains by UNSM treatments.