Praseodymium (III) and dysprosium (III) isonicotinamide (INA) complexes grafted onto modified mesoporous MCM-41 with 3-chloropropyltriethoxysilane (CPTES)), as two novel catalysts, were synthesized. The catalysts were determined using SEM, Mapping, EDX, FT-IR, TGA, XRD, ICP, and BET analysis. The catalysts (MCM-41- INA-Pr and MCM-41-INA-Dy) were further studied for the oxidation reaction of sulfur-containing compounds. Catalytic results displayed that the MCM-41-INA-Pr and MCM-41-INA-Dy show high effectiveness for promoting the oxidation reaction of sulfur-containing compounds. The catalysts could be recycled for seven runs with negligible destruction of catalytic performance.