Supported undecamolybdophosphate was synthesized and characterized by various physicochemical techniques and successfully used for solvent free oxidation of styrene and of benzyl alcohol to benzaldehyde. Influence of the reaction parameters (molar ratio of substrate to H2O2, amount of the catalyst, reaction time, and reaction temperature) were studied. The catalyst was reused three times without any significant loss in the catalytic activity. FT-IR, XRD, and DRS of regenerated catalyst indicated that the catalyst was undegraded and stable after the reaction. The novelty of the work lies in obtaining a single selective product, benzaldehyde, as well as a high TON for the same, under mild conditions.