In this study, we investigate the atomic layer deposition (ALD) process on all-inorganic CsPbBr3 perovskite nanocrystals (PNCs) to introduce an inorganic electron transport layer (ETL) in light-emitting diode (LED) devices. Two types of CsPbBr3 PNCs were synthesized with oleate (OA) and oleylammonium (OLA) ligands on the surface. We found that CsPbBr3 PNCs with Cs oleate surfaces experienced severe photoluminescence (PL) quenching after the ALD process, while those with oleylammonium bromide surfaces did not show any significant PL drop. Transmission electron microscopy and X-ray photoelectron spectroscopy revealed that significant Pb metal formation and Ruddlesden-Popper planar faults, linked to uncoordinated Pb2+ ion defects, were generated in CsPbBr3 PNCs terminated with Cs oleate after ALD ZnO. Finally, we fabricated LEDs using PNCs with an ALD ZnO process to introduce inorganic ZnMgO nanoparticles as the ETL. The devices processed with ALD exhibited superior luminance and external quantum efficiency compared to those without the ALD process. This research provides crucial insights into the surface-dependent chemistry of PNCs and the surface-dependent performance of perovskite-based optoelectronic devices.