High-energy-emitting CsPbCl3 nanocrystals have shown significant loss and enhancement of their emission intensity (∼40-50 folds) during purification and surface treatments, respectively. This confirms that the surfaces of these nanocrystals are very sensitive. In this Letter, physical insights of the interface bindings on the surface of these blue-emitting CsPbCl3 nanocrystals with different passivating agents and their consequential impact on purification are investigated. Using various metal chlorides irrespective of the charge and size of the metal ions, metal acetates, and nonmetal chloride, the predominant influence of chloride ions in helping retrieve/intensify the blue emission is established. The purification processes are observed to be very delicate, and successive purifications with introduction of polar nonsolvents led to the transformation of an emitting cubic CsPbCl3 phase to nonemitting tetragonal CsPb2Cl5 phase nanocrystals irreversibly. The impact of various salt additions only temporarily helped in enhancing the emission, but the phase change remained inevitable upon successive purification. However, as a remedy, by in situ use of alkylammonium chloride salt in high-temperature reactions, the surface binding was improved, and significant emission as well as the phase could be retained with successive purifications.