The fabrication of reusable and biodegradation materials from renewable resources such as cellulose is essential for a sustainable world. The core-shell structured CdS-decorated TiO2/Carbon microspheres (CdS/TiO2/Carbon MS) photocatalyst was synthesized with controlled hydrolysis and a novel sonochemical method. It was prepared by using crosslinked microcrystalline cellulose as the core, tetrabutyl titanate as the titania source and CdS as the photosensitizer. The morphology, chemical structure and properties of the obtained material were characterized by many means. Additionally, the photocatalytic activity of the CdS/TiO2/Carbon MS was evaluated by the photodegradation efficiency of Rhodamine B solution, which reached 95.24% under visible light irradiation. This study demonstrated the excellent photocatalytic performance of CdS/TiO2/Carbon MS, which might have promising applications in environmental treatments.