A method to suppress the photocorrosion of ZnO nanoparticles was developed by surface hybridization of ZnO with graphite-like carbon layers. The presence of carbon on the surface of the ZnO could significantly suppress the coalescence and crystal growth of ZnO nanoparticles during high-temperature treatment. The nanosized structure of ZnO was well preserved even after high-temperature calcination. The photocatalytic activity of ZnO was enhanced by hybridization with carbon layers attributed to the improved adsorption ability and crystallinity. The as-prepared samples exhibited high activity even after 720 h of photocatalysis reaction, while the pure ZnO nanoparticle was almost deactivated in 100 h due to serious photocorrosion. The as-prepared samples also showed much better activity under extreme pH conditions than that of pure ZnO. The mechanism of photocorrosion suppression and higher stability was then systematically investigated based on the crystal structure and the photocatalysis degradation process.