Mg alloys are widely used in aerospace and electronics owing to their excellent mechanical and physical properties. However, their utility is hindered by poor tribology and corrosion resistance. This study indicates the efficacy of employing highly hydrophobic "spherical micro-/nanostructures" comprising α-Al2O3/ZrO2 particles, prepared using combustion-synthesis-assisted water atomization and chemical modification methods, along with a one-step spray coating process (epoxy resin (EP)/(α-Al2O3/ZrO2)). This approach notably enhances the corrosion resistance and friction performance of Mg alloys. The study delves into evaluating the tribological properties and corrosion resistance of EP/(α-Al2O3/ZrO2) coatings and Mg alloys with different α-Al2O3/ZrO2 contents under simulated body fluid conditions. At 102 wt % α-Al2O3/ZrO2 content, the nanocomposite coating reaches a surface WCA of 145°, reduces the friction coefficient to 0.087, and exhibits the lowest self-corrosion current alongside the highest self-corrosion potential. The investigation underscores that the combined effect of α-Al2O3/ZrO2 particles in a 102 wt % nanocomposite coating improves the hydrophobicity, friction, and corrosion resistance of Mg alloys, thus broadening their scope of applications.