Oxo-transfer reactions of a variety of substrates in DMF or methanol using polymer-supported molybdenyl thioglycolate (PSMT) have been investigated. The clean oxidation of Me2PhP, n-butanethiol or benzoin to yield Me2PhPO, disulfide or benzil, respectively, occurs in high yield. In the presence of air or pyridine N-oxide, a catalytic cycle is accomplished which goes on until the completion of the substrate.