Shelling with chalcogenides on the surface of lead halide perovskite (LHP) nanocrystals (NCs) is believed to be an effective approach to increase their stability under high-moisture/aqueous conditions, which is important for LHP NC-based optoelectronic devices. However, it is still a challenge to prepare high-quality LHP/chalcogenide core/shell NCs with moisture/aqueous stability. In this work, a surface-defect-induced strategy is carried out to facilitate the adsorption of Br- ions and subsequently Zn2+ ions to preform a bipolar surface, which reduces the energy barrier at the CsPbBr3/ZnS interface and promotes the epitaxial growth of the ZnS shell layer. The aqueous stability of the as-received NCs shows an increase of over 12 times compared to that of the original one. Likewise, Mn2+ ions are introduced to further reduce the geometric symmetry mismatch and defect density at the CsPbBr3/ZnS interface. Interestingly, aqueous stability characterizations illustrate negligible degradation even after 230 min of ultrasonication, suggesting their outstanding stability. This work proposes an effective approach to prepare high-quality LHP/chalcogenide core/shell NCs, which possess great potential in the fabrication of stable optoelectronic devices.