Halide vacancies cause lattice degradation and nonradiative losses in halide perovskites. In this study, we strategically fill bromide vacancies in CsPbBr 3 perovskite nanocrystals with NaBr, KBr, or CsBr at the organic− aqueous interface for hydrophobic ligand-capped nanocrystals or in a polar solvent (2-propanol) for amphiphilic ligand-capped nanocrystals. Energydispersive X-ray spectra, powder X-ray diffraction data, and scanning transmission electron microscopy images help us confirm vacancy filling and the structures of samples. The bromide salts increase the photoluminescence quantum yield (98 ± 2%) of CsPbBr 3 by decreasing the nonradiative decay rate. Single-particle studies show the quantum yield increase originates from the poorly luminescent nanocrystals becoming highly luminescent after filling vacancies. Furthermore, we tune the optical band gap (ultraviolet−visible− near-infrared) of the hydrophobic ligand-capped nanocrystals by halide exchange at the toluene−water interface using saturated NaCl or NaI solutions, which completes in about 60 min under continuous mixing. In contrast, the amphiphilic ligand accelerates the halide exchange in 2-propanol, suggesting ambipolar functional groups speed up the ion-exchange reaction. The bromide vacancy-filled or halide-exchanged samples in a toluene−water biphasic solvent show higher stability than amphiphilic ligand-capped samples in 2-propanol. This strategy of defect passivation, ion exchange, and ligand chemistry to improve quantum yields and tune band gaps of halide perovskite nanocrystals can be promising for designing stable and water-soluble perovskite samples for solar cells, light-emitting diodes, photodetectors, and photocatalysts.