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Intelligent surfaces with controlled wettability have caught much attention in industrial oily wastewater treatment. In this study, a hygro-responsive superhydrophilic/underwater superoleophobic coating was fabricated by the liquid-phase deposition of SiO₂ grafted with perfluorooctanoic acid. The wettability of the surface could realize the transformation from superhydrophilicity/underwater superoleophobicity (SHI/USOB) to superhydrophobicity/superoleophilicity (SHB/SOI), both of which exhibited excellent separation performance towards different types of oil–water mixtures with the separation efficiency higher than 99%. Furthermore, the long-chain perfluoroakyl substances on the surface could be decomposed by mixing SiO₂ with TiO₂ nanoparticles under UV irradiation, which could reduce the pollution to human beings and environment. It is anticipated that the prepared coating with controlled wettability could provide a feasible solution for oil–water separation.