This study presents a chelation-directed interface engineering approach to create self-cleaning membranes for efficient water treatment. The researchers designed a metal-polyphenol network to direct the armorization of catalytic nanofilms on inert polymeric membranes, resulting in a highly polarized, superhydrophilic, and ultralow-adhesion membrane that enables efficient crude oil-in-water emulsion separation. The membrane exhibits a flux recovery rate exceeding 99.9%, significantly outperforming traditional cleaning methods. The chelation-directed nanoarmored membrane shows a 48-fold and 6.8-fold improvement in self-cleaning regeneration compared to control membranes and simple hydraulic cleaning, respectively. Density functional theory calculations reveal strong precursor interactions, contributing to the membrane's stability and performance. The membrane's superhydrophilic and superoleophobic properties enable effective fouling prevention and in-place self-cleaning. The study highlights the potential of this approach for sustainable applications in catalysis, biomedicine, environmental remediation, and beyond. The method is simple, mild, and green, offering a promising solution for energy-efficient water treatment and practical water-remediation applications. The membrane demonstrates excellent stability under various conditions, including acid/alkali, saturated NaCl solution, and repeated bending. The results show that the chelation-directed mineralization strategy is effective for creating high-performance self-cleaning membranes with superior separation efficiency and regeneration capacity. The study provides a route for the eco-friendly construction of active catalytic self-cleaning membranes for energy-efficient water treatment.This study presents a chelation-directed interface engineering approach to create self-cleaning membranes for efficient water treatment. The researchers designed a metal-polyphenol network to direct the armorization of catalytic nanofilms on inert polymeric membranes, resulting in a highly polarized, superhydrophilic, and ultralow-adhesion membrane that enables efficient crude oil-in-water emulsion separation. The membrane exhibits a flux recovery rate exceeding 99.9%, significantly outperforming traditional cleaning methods. The chelation-directed nanoarmored membrane shows a 48-fold and 6.8-fold improvement in self-cleaning regeneration compared to control membranes and simple hydraulic cleaning, respectively. Density functional theory calculations reveal strong precursor interactions, contributing to the membrane's stability and performance. The membrane's superhydrophilic and superoleophobic properties enable effective fouling prevention and in-place self-cleaning. The study highlights the potential of this approach for sustainable applications in catalysis, biomedicine, environmental remediation, and beyond. The method is simple, mild, and green, offering a promising solution for energy-efficient water treatment and practical water-remediation applications. The membrane demonstrates excellent stability under various conditions, including acid/alkali, saturated NaCl solution, and repeated bending. The results show that the chelation-directed mineralization strategy is effective for creating high-performance self-cleaning membranes with superior separation efficiency and regeneration capacity. The study provides a route for the eco-friendly construction of active catalytic self-cleaning membranes for energy-efficient water treatment.