Edge‐Stitched Lamellar Metal–Organic Framework Membranes for Resilient and Selective Water Purification

ABSTRACT Reliable water purification demands membranes that simultaneously offer high selectivity and fouling resistance within complex matrices. While lamellar metal–organic framework (MOF) membranes are promising, achieving structural stability without compromising surface functionality remains a challenge. Here we bridge this gap by introducing an edge‐stitched laminar MOF membrane fabricated using a molecular stitching‐interfacial polymerization (MS‐IP) strategy. By directing the confined reaction of piperazine within the lateral gaps of stacked MOF nanosheets, we engineer polyamide nanodomains that seal lamellar defects while facilitating high MOF surface exposure. This architecture creates a microscale hydrophilic‐hydrophobic heterogeneous interface that stabilizes a robust hydration layer, effectively repelling foulant adhesion. The edge‐stitched MOF membranes achieve >89% removal efficacy of diverse per‐ and polyfluoroalkyl substances (PFAS) at a high water permeance of 25.6 L m −2 h −1 bar −1 . Furthermore, the membrane demonstrates exceptional durability during 30 days of raw river water filtration. This structural‐interfacial design provides a versatile framework for developing resilient, high‐performance membranes for sustainable water treatment.