A green polyol-reduction approach was employed to load Cu onto the surface of oxide semiconductors (WO3, TiO2, CeO2) for improved wastewater remediation. All of the composites exhibited removal enhancement for CR dye through adsorption-photocatalysis synergy, instead of a single adsorption mode. The decoration of copper particles not only affects the ;-potential, surface wettability, and the corresponding adsorption capacity but also has a significant impact on the interface charge separation during the photocatalysis process. Indeed, the Cu-WO3 hybrids displayed positive charge and relatively poor hydrophilic property, which contributes to its superior adsorption capability toward a CR dye molecule. At the same time, compared with pure WO3, the recombination of photoinduced electrons and holes reduced and interfacial charge transfer between Cu and WO3 was significantly enhanced, which greatly promoted the CR photodegradation. This adsorption-photocatalysis synergy toward a CR dye solution remediation through surface/interface engineering was also confirmed by Cu-TiO2 and Cu-CeO2 hybrids.