Titanium nanotubes were hydrothermally synthesized via a two-step method for ODS (oxidative desulfurization). The catalysts’ structures were characterized by XRD (X-ray diffraction), FT-IR, UV-Vis (UV-Vis diffuse reflectance spectra), NH3-TPD, etc. The effects of O/S molar ratio and catalyst dosage, etc., were systematically investigated. The catalyst exhibited remarkable performance, so that the removal of DBT (dibenzothiophene) was nearly 100% under the optimal conditions in 10 min. Also, the catalysts could be easily reused for six consecutive cycles. The hydrogen-assisted thermocatalytic mechanism over titanium nanotubes for ODS was also studied and an effective reactant concentration (ERC) number of 70.8 was calculated.