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Dye sensitization represents a promising route to address the limited photoabsorption in semiconductor photocatalysis. However, efficient water purification using dye-sensitized photocatalysts has remained an unmet challenge. Here we report a novel strategy to promote dye-sensitized photocatalysis by combining the advantages of interfacial Fenton reaction construction and air-liquid-solid triphase contact. An alveoli-like Janus membrane was developed with bilayer electrospun micro/nanofibers, where the outer layer is hydrophilic semiconductor catalyst sensitized by an iron (II) phthalocyanine (FePc) photosensitizer, which can also act as the trigger of H2O2 activation; the hydrophobic internal layer serves as a gas passage to deliver O2 from air to the catalytic interface, boosting the photoinduced electrons conversion and H2O2 generation. This architecture allows a superior level of photosensitizer decoration when using TiO2 as the model semiconductor catalyst, which corresponds to highly efficient activity for photodegradation of organic contaminations accompanied with a high apparent quantum yield at around 660 nm. Our work may provide new insights into the development of high-efficiency solar driven photocatalysts for widespread applications.