CuO nanosheets were deposited on the surface of TiO2 nanotube arrays by a SILAR method. The visible light photocurrent density of TiO2 NTs/CuO (M) was 19.81 mA/cm2, the photovoltage was −0.59 V/cm2, the flat band was −0.53 V, and the carrier concentration was 5.57 × 1019 cm−3. The TiO2 NTs/CuO (M) showed the optimal photoelectrocatalytic removal efficiencies of methyl orange, rhodamine B, methyl blue and Cr(VI). Display omitted •CuO nanosheets were deposited on TiO2 nanotube arrays by a SILAR method.•The TiO2 NTs/CuO (M) photoelectrode showed the excellent photoelectrochemical properties.•The PEC mechanism of TiO2 NTs/CuO photocatalysts was proposed. The CuO nanosheets were deposited on the surface of TiO2 nanotube arrays (TiO2 NTs/CuO) by the successive ionic layer adsorption and reaction (SILAR) method at 90 °C. The results indicated that the reactant concentration influenced the morphology, visible light response and corresponding photoelectrochemical performances of TiO2 NTs/CuO. The TiO2 NTs/CuO (M) prepared in 0.04 mol/L of Cu2+ solution possessed the highest visible light photocurrent (19.81 mA/cm2), photovoltage (−0.59 V/cm2) and charge carrier concentration (5.57 × 1019 cm−3) among these photoelectrodes. Beside, the TiO2 NTs/CuO (M) photoelectrode could achieve rapid pollutant removal, and the photoelectrocatalytic (PEC) efficiencies for RhB, MO, MB and Cr(VI) were 55.36%, 48.28%, 89.61% and 74.76% under solar irradiation, respectively. Hence, the novel TiO2 NTs/CuO (M) photoelectrode would exhibit excellent property in the applications of solar cells and photocatalysts.