The present study reports on the origins of room temperature ferromagnetism in zinc oxide (ZnO)-Al nanoparticles using a combination of X-ray absorption near edge structure (XANES) experiments and density functional theory (DFT) simulations. Our findings reveal that the spontaneous magnetization observed in these systems originates from the adsorption of Al on surfaces of ZnO nanoparticles. Our DFT simulations have identified unique configurations for Al adsorption on ZnO surfaces that lead to a spin-polarized charge transfer to O 2p states in surface and subsurface layers. XANES spectra of the magnetic ZnO/Al nanoparticles provide the necessary experimental evidence for the charge transfer to ZnO surfaces and confirm the origin of ferromagnetic behavior. Our results illustrate a complex interplay between the atomic level interfacial structure and the resulting ferromagnetic ordering in metal-coated semiconductor oxide nanostructures.