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Hydrogel coatings that can endow various substrates with superior properties (e.g., biocompatibility, hydrophilicity, and lubricity) have wide applications in the fields of oil/water separation, antifouling, anti-bioadhesion, etc. Currently, the engineering of multifunctional hydrogel-coated materials with superwettability and water purification property using a simple and sustainable strategy is still largely uninvestigated but has a beneficial effect on the world. Herein, we successfully prepared poly(2-acrylamido-2-methyl-1-propanesulfonic acid) hydrogel/β-FeOOH-coated poly(vinylidene fluoride) (PVDF/PAMPS/β-FeOOH) membrane through free-radical polymerization and the in situ mineralization process. In this work, owing to the combination of hydrophilic PAMPS hydrogel coating and β-FeOOH nanorods anchored onto PVDF membrane, the resultant PVDF/PAMPS/β-FeOOH membrane achieved outstanding superhydrophilicity/underwater superoleophobicity. Moreover, the membrane not only effectively separated surfactant-stabilized oil/water emulsions, but also possessed a long-term use capacity. In addition, excellent photocatalytic activity against organic pollutants was demonstrated so that the PVDF/PAMPS/β-FeOOH membrane could be utilized to deal with wastewater. It is envisioned that these hydrogel/β-FeOOH-coated PVDF membranes have versatile applications in the fields of oil/water separation and wastewater purification. [ABSTRACT FROM AUTHOR]