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Selective photooxidation of toluene to benzaldehyde using O2 as an oxidant has the advantages of mild reaction conditions and excellent atomic economy, but it often suffers from low conversion efficiency. To promote the photooxidation process, we fabricated iron-doped Bi2WO6 microflowers by a simple hydrothermal method to boost the formation of oxygen vacancies. The rich presence of oxygen vacancies not only accelerates the separation of photogenerated charge carriers but also enhances O2 activation for ·O2 – generation. Besides the slight improvement of Bi2WO6 stability, the Fe-doped Bi2WO6 displays enhanced activity and selectivity for benzaldehyde generation from toluene under visible light. This work illustrates a simple strategy for successful modulation of Bi2WO6 for improved performance in the photocatalytic selective oxidation processes.