Functional mesoporous Mo-SiO2 materials were synthesized by a one-pot and facile room-temperature procedure, and characterized by X-ray diffraction, TEM, Raman spectroscopy, FT-IR, diffuse reflectance spectra, and BET analysis. The experimental results demonstrated that the mesoporous materials presented a high dispersion of molybdenum species and excellent catalytic activity for the removal of dibenzothiophene (DBT) without organic solvents as extractants. The catalytic performance on different sulfur-containing compounds was also investigated in detail. After recycling for eight times, the removal of the oxidation desulfurization system could still reach high values. GC-MS analysis detected the oxidation product of DBT. A mechanism was proposed for the absorptive oxidation process of sulfur compounds.