In the present investigation, we exploited the visible region absorbance (λ > 380 nm) of uranyl ions anchored onto mesoporous MCM-41 matrix for the vapor-phase photooxidation of volatile organic compounds (VOCs) such as benzene, toluene, cyclohexane, cyclohexene, and o- xylene. In all cases, the only complete oxidation products, viz., carbon dioxide and water, were obtained. Further, the extent of conversion to carbon dioxide depended upon the nature of the organic compound. Under sunlight, the uranyl-anchored catalyst was found to be highly active for the degradation of a stable molecule like benzene, though longer irradiation times were needed for its complete conversion. This study signifies the potential applicability of the uranyl- anchored photocatalyst for applications related to air cleaning under ambient conditions of solar radiation and air.