Photocatalytic oxidation of alcohols with high selectivity is a promising approach for the synthesis of organic compounds under mild conditions and for solar energy conversion. In this work, we report on the highly selective anaerobic photooxidation of alcohols to carbonyl compounds with coupled H2 production over Pt‐loaded Fe‐doped SrTiO3 under visible light. Representatively, an optimized apparent quantum efficiency of 13.2 % at 420 nm was obtained for benzyl alcohol oxidation. X‐ray absorption fine structure and in situ diffuse reflectance IR spectroscopy revealed that the surface oxygen vacancies and the fine‐tuned valence band edge position induced by Fe doping not only contributed to the activation of α‐C−H bonds in alcohols, but also avoided the over‐oxidation of the obtained carbonyl compounds.