Phosphorus slag (P-slag) as a cost-effective source is used for the extraction of mesoporous silica SiO 2 . The composite materials of the Keggin-type heteropolyanions (HPAs) were anchored on SiO 2 and successfully prepared via an impregnation approach. Various approaches including X-ray diffraction, Brunauer−Emmett−Teller, inductively coupled plasma, field emission scanning electron microscopy-energy dispersive spectrum, ultraviolet−visible, temperature-programmed desorption, Fourier transform infrared, and transmission electron microscopy were employed to characterize the samples. HPAs supported on SiO 2 were employed for the oxidation of organic sulfur compounds [e.g., benzothiophene (BT), dibenzothiophene (DBT), and 4,6dimethyldibenzothiophene (4,6-DMDBT)] from the model fuel. HPA-loaded SiO 2 catalysts illustrated outstanding catalytic activity in the oxidative desulfurization procedure. The removal performance of the DBT using Cs 2 W 9 V 3 /SiO 2 was greater than that using other materials under the optimum condition. The maximum level of DBT removal by Cs 2 W 9 V 3 /SiO 2 reached 100%. The removal performance of various substrates followed the order DBT > 4,6-DMDBT > BT. The Cs 2 W 9 V 3 -incorporated SiO 2 catalyst illustrated brilliant reusability five times with negligible reduction in performance. Besides, the kinetic studies exhibited that the desulfurization procedure on DBT-containing sulfur compound verified a pseudo-first-order kinetic model. The Arrhenius activation energy for the Cs 2 W 9 V 3 /SiO 2 catalyst obtained 47.2 kJ/mol.