A new greener strategy to incorporate Bi 2 S 3mercaptopropionic acid (MPA) quantum dots (QDs) onto TiO 2 nanotube (NT) films was developed, using in situ electrochemical synthesis with a graphite/sulfur powder macroelectrode (cathode) and cavity cell. Simultaneously, the obtained QDs were adsorbed on TiO 2 NTs, for the photoelectrochemical cell (PEC) assays. After the electrochemical synthesis, different thermal post-treatments were performed for growth and crystallization of obtained nanocrystals. The obtained TiO 2 −Bi 2 S 3 nanostructured composites were characterized by UV−vis, diffuse reflectance spectroscopy, X-ray diffraction, scanning electron microscopy and transmission electron microscopy. Photoelectrochemical tests were carried out, where TiO 2 NTs/Bi 2 S 3 QDs with 15 min post-treatment at 90 °C presented a greater photocurrent density, when irradiated with visible light (427−655 nm region, 10 mW.cm −2 ) and compared to pristine TiO 2 NTs. Such performance can be attributed to the synergetic effect caused by the good interface between TiO 2 NTs/Bi 2 S 3 QDs, promoted by the electrochemical method of synthesis employed. The proof of concept evidenced in this work can be potentially extended for the sensitization of TiO 2 NTs with other semiconductors for PEC hydrogen generation and solar cell applications.