AgBr-BiOBr microspheres assembled by nanosheets were prepared on the surface of TiO2 nanotube arrays (TiO2 NTs/AgBr/BiOBr) by the solvothermal deposition using CTAB as the bromine resource and morphology controlling agent. The TiO2 NTs/AgBr/BiOBr significantly extended light response to the visible light region, and showed excellent visible light photocurrent, photovoltage, interface impedance, carrier concentration and photoelectrocatalytic removal of pollutants. The results indicated that TiO2 NTs/AgBr/BiOBr (0.30) prepared with 0.30 g of CTAB showed the optimal photoelectrochemical performances. The photoelectrocatalytic mechanism about electron transfer and active groups for the decomposition of organic dyes was tentatively proposed. The new hybrid photoelectrode provides promising guidelines for the preparation of sensitizers with effective visible light harvesting and photoelectrochemical activities.