AbstractIn this work, CdS sensitized TiO2 nanotube arrays (CdS/TiO2NTs) electrode was synthesized with the CdS deposition on the highly ordered titanium dioxide nanotube arrays (TiO2NTs) by sequential chemical bath deposition method (S‐CBD). The as‐prepared CdS/TiO2NTs was characterized by field‐emission scanning electron microscopy (FE‐SEM) and X‐ray diffraction (XRD). The results indicated that the CdS nanoparticles were effectively deposited on the surface of TiO2NTs. The amperometric I‐t curve on the CdS/TiO2NTs electrode was also presented. It was found that the photocurrent density was enhanced significantly from 0.5 to 1.85 mA/cm2 upon illumination with applied potential of 0.5 V at the central wavelength of 253.7 nm. The photoelectrocatalytic (PEC) activity of the CdS/TiO2NTs electrode was investigated by degradation of methyl orange (MO) in aqueous solution. Compared with TiO2NTs electrode, the degradation efficiencies of CdS/TiO2NTs electrode increased from 78% to 99.2% under UV light in 2 h, and from 14% to 99.2% under visible light in 3 h, which was caused by effective separation of the electrons and holes due to the effect of CdS, hence inhibiting the recombination of electron/hole pairs of TiO2NTs.