The development of efficient charge transport layers is crucial for realizing high-performance and stable quantum dot light-emitting diodes (QD-LEDs). The use of a ZnO/ZnMgO bilayer as an electron transporting layer (ETL) has garnered considerable attention. This configuration leverages the high electron mobility of ZnO and the favorable surface state of ZnMgO. Furthermore, the versatility of this configuration extends to its wide range of thickness tunability, rendering it suitable for the construction of thick devices for top-emitting structures with microcavities. However, despite the promising attributes of this bilayer configuration, the impact of the ZnO/ZnMgO bilayer ETL interface on QD-LEDs performance remains largely unexplored. Thus, this study investigated the effect of ultraviolet ozone (UVO) treatment on the stabilization of the ZnO/ZnMgO interface. UVO treatment was found to significantly enhance luminance uniformity across the QD-LEDs emission area while improving operational stability by over 4-fold. Comprehensive analyses employing X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy confirmed that UVO treatment significantly reduced the defect states of the hydroxyl groups and removed the insulating native ethanolamine ligands, thereby facilitating improved and uniform electron transport. Moreover, the effectiveness of UVO treatment in enhancing electron transport was supported by impedance analyses. Therefore, this paper presents an effective approach for enhancing the interface of a highly potent ZnO/ZnMgO bilayer ETL, which can ultimately improve the luminance uniformity and stability of QD-LEDs.