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Bimetallic Pd-Fe catalysts supported on TiO 2 are shown to be highly effective toward the selective oxidation of benzyl alcohol to benzaldehyde via the in situ production of H 2 O 2 from molecular H 2 and O 2 , under conditions where no reaction is observed with molecular O 2 alone. The rate of benzyl alcohol oxidation observed over supported Pd-Fe nanoparticles is significantly higher than those of either Pd-Au or Pd-only analogues. This enhanced activity can be attributed to the bifunctionality of the Pd-Fe catalyst to both synthesize H 2 O 2 and catalyze the production of oxygen-based radical specie,s as indicated by an electron paramagnetic resonance analysis. Further studies also reveal the noninnocent nature of the solvent, resulting in the propagation of radical generation pathways.