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A novel (CdS-Mn/MoS/CdTe)-sensitized TiO nanotube arrays (NTAs) photoelectrode has been prepared by electrodeposite, successive ionic layer adsorption and reaction (SILAR) coupled with hydrothermal method. When a ZnS layer was added on the top of CdS-Mn/MoS/CdTe/TiO, a notable red-shift and high absorption was observed in the visible light region. The photocurrent density (mA/cm) systematically increases from TiO NTAs (0.43), CdTe/TiO (1.09), MoS/CdTe/TiO (1.80), CdS-Mn/MoS/CdTe/TiO (2.40), to ZnS/CdS-Mn/MoS/CdTe/TiO (3.41) under visible light irradiation, due to the type-II semiconductor heterostructures comprising multiple components with a staggered band offset. Such a heterostructure possesses an enhanced photocatalytic performance towards degradation of organic contaminant, e.g. P-Nitrophenol (PNP) and Rhodamine B (RhB).