In this work, the capping layer atop anodic TiO 2 nanotube arrays (NTAs), which hinders filling of other guest materials and transport of charge carriers, is discerned to be TiO 2 nanotapes. Then, it is completely removed by a novel sonication-polishing (SP) treatment, after which Sb 2 S 3 is subsequently introduced to fill the nanotubes by chemical bath deposition. The morphological, structural, and optical properties of the SP-treated TiO 2 NTAs and TiO 2 NTAs/Sb 2 S 3 heterogeneous structures are characterized systematically. The results indicate that SP treatment opens the tops of nanotubes with diameters of ∼120 nm, which endure a phase conversion from amorphous to anatase after calcination at 450°C; besides, stibnite Sb 2 S 3 with a band gap of ∼1.75 eV inside the TiO 2 networks is formed upon heat treatment at 330°C in Ar, which enhances the absorption in visible light range. The photoelectrochemical (PEC) and photovoltaic properties for the SP-treated TiO 2 NTAs are investigated. Results shows that the photoresponse of TiO 2 NTAs is improved by the SP treatment, and the photocurrent for the TiO 2 NTAs/Sb 2 S 3 electrode is substantially enhanced as compared to the bare TiO 2 one. A high efficiency of 6.28 % is achieved in a TiO 2 NTAs/Sb 2 S 3 PEC cell. In addition, charge recombination in the photoanode of dye-sensitized solar cells (DSSCs) is observed to be greatly retarded by using the SP-treated TiO 2 NTAs as compared to TiO 2 nanoparticles (NPs). Thus, the SP anodic TiO 2 NTAs are promising in applications in various PEC areas such as photocatalysis and sensitized solar cells.