Mesoporous Al-MCM-41@Ag/TiO2 nanocomposites were synthesized successfully by combining the sol-gel method and hydrothermal treatment, using titanium isopropoxide (TTIP), AgNO3, and Vietnamese bentonite as precursors of Ti, Ag, and Si, respectively. The synthesized materials were well characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N2 adsorption-desorption isotherm measurements, energy dispersive X-ray spectroscopy (EDX), UV-visible diffuse reflectance spectroscopy (UV-Vis/DRS), and X-ray photoelectron spectroscopy (XPS). The photocatalytic activity was evaluated by the photodegradation of dibenzothiophene (DBT) under both UV and visible light irradiation. MCM-41@Ag/TiO2 catalyst exhibited high catalytic activity for the oxidative desulfurization (ODS) of DBT reaching almost 100% conversions at 50°C after 2 h under UV and visible light irradiations. The significant enhanced degradation of DBT over Al-MCM-41@Ag/TiO2 might be due to the synergy effects of high surface area of MCM-41, well-distributed TiO2 anatase, and reduced electron-hole recombination rates due to the dispersion of Ag nanoparticles.