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However, conventional nanofiltration (NF) membranes, which rely primarily on charge\u2010based exclusion, often struggle to achieve efficient separation of counter\u2010ions, limiting their applicability. Herein, we report a composition\u2010regulated zwitterionic copolymer grafting strategy that enables precise tuning of membrane surface chemistry and pore structure of NF membranes. A zwitterionic copolymer, poly(2\u2010methacryloyloxyethyl phosphorylcholine\u2010co\u20102\u2010aminoethyl methacrylate hydrochloride) (P(MPC\u2010co\u2010AEMA)), with tunable MPC\/AEMA ratios, is grafted onto the polyamide (PA) selective layer via secondary interfacial polymerization. Rather than relying solely on the introduction of zwitterionic functionalities, this approach leverages the balance between reactive anchoring segments (AEMA) and zwitterionic segments (MPC) to regulate grafting density, surface charge, and structural evolution of the PA layer. Through systematic control of copolymer composition, the membrane properties can be finely tuned from strongly charged to near\u2010neutral surfaces with concurrently reduced pore size, thereby suppressing charge\u2010sign\u2010dependent electrostatic interaction effects and promoting sterically governed ion transport. This work demonstrates that balancing reactive anchoring and zwitterionic segments offers a rational strategy for tuning membrane physicochemical properties and advancing NF membranes toward charge\u2010sign\u2010independent ion\u2010selective separations.<\/jats:p>","DOI":"10.1002\/advs.77377","type":"journal-article","created":{"date-parts":[[2026,8,25]],"date-time":"2026-08-25T15:03:17Z","timestamp":1787670197000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Precise Control of Charge\u2013Structure Coupling in Polyamide Membranes for Mono\u2010 and Divalent Ion Separation"],"prefix":"10.1002","author":[{"given":"Shaofan","family":"Duan","sequence":"first","affiliation":[{"name":"Research Center for Membrane and Film Technology Kobe University  Nada Kobe Japan"},{"name":"Department of Chemical Science and Engineering Kobe University  Nada Kobe 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