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Industrial translation of pressure\u2010resistant mixed matrix membranes (MMMs) is largely impeded by the dispersion instability of nanofillers under rapid, non\u2010equilibrium manufacturing conditions, which leads to uncontrollable aggregation and interfacial defects during processing. Here, we present a universal \u201cpre\u2010occupation and post\u2010activation\u201d strategy to construct positively charged polymer\u2010brush metal\u2013organic frameworks (MOFs). This approach endows the fillers with a dual\u2010stabilization mechanism: electro\u2010steric effects ensure static dispersion stability, while a hydrogen\u2010bonding\u2010driven interfacial interlocking mechanism maintains stability during dynamic processing. Together, these mechanisms synergistically facilitate the seamless integration of nanofillers within ultrathin selective layers. This design allows roll\u2010to\u2010roll production of 1 m\u2010wide, pressure\u2010resistant mixed matrix composite membranes (MMCMs) with tunable CO\n                    <jats:sub>2<\/jats:sub>\n                    separation performance. The resulting MMCMs deliver outstanding CO\n                    <jats:sub>2<\/jats:sub>\n                    \/CH\n                    <jats:sub>4<\/jats:sub>\n                    and CO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    separation under industrially relevant pressures, reducing the required membrane area by more than an order of magnitude compared with laboratory\u2010scale membranes. A spiral\u2010wound module with an effective area of 0.4\u20132 m\n                    <jats:sup>2<\/jats:sup>\n                    further validates the scalability and operational robustness. This work overcomes a long\u2010standing barrier in MMM processing, marking a significant step toward industrial implementation of MOF\u2010based, energy\u2010efficient gas separation technologies.\n                  <\/jats:p>","DOI":"10.1002\/adma.202520099","type":"journal-article","created":{"date-parts":[[2026,3,8]],"date-time":"2026-03-08T23:08:51Z","timestamp":1773011331000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Positively Charged Polymer\u2010Brush MOFs for Large\u2010Area, Pressure\u2010Resistant Gas Separation Membranes"],"prefix":"10.1002","volume":"38","author":[{"given":"Yi","family":"Yang","sequence":"first","affiliation":[{"name":"Chemical Engineering Research Center Tianjin Key Laboratory of Membrane Science and Desalination Technology Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) State Key Laboratory of Chemical Engineering and Low\u2010Carbon Technology (Tianjin University) School of Chemical Engineering and Technology Tianjin University Tianjin China"},{"name":"Haihe Laboratory of Sustainable Chemical Transformations  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ye","family":"Yuan","sequence":"additional","affiliation":[{"name":"Chemical Engineering Research Center Tianjin Key Laboratory of Membrane Science and Desalination Technology Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) State Key Laboratory of Chemical Engineering and Low\u2010Carbon Technology (Tianjin University) School of Chemical Engineering and Technology Tianjin University Tianjin China"},{"name":"Haihe Laboratory of Sustainable Chemical Transformations  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxiu","family":"Sun","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Technology Tiangong University  Tianjin 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University) School of Chemical Engineering and Technology Tianjin University Tianjin China"},{"name":"Haihe Laboratory of Sustainable Chemical Transformations  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weifan","family":"Wang","sequence":"additional","affiliation":[{"name":"Chemical Engineering Research Center Tianjin Key Laboratory of Membrane Science and Desalination Technology Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) State Key Laboratory of Chemical Engineering and Low\u2010Carbon Technology (Tianjin University) School of Chemical Engineering and Technology Tianjin University Tianjin China"},{"name":"Haihe Laboratory of Sustainable Chemical Transformations  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qinghua","family":"Li","sequence":"additional","affiliation":[{"name":"Chemical Engineering Research Center Tianjin Key Laboratory of Membrane Science and Desalination Technology Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) State Key Laboratory of Chemical Engineering and Low\u2010Carbon Technology (Tianjin University) School of Chemical Engineering and Technology Tianjin University Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Menglong","family":"Sheng","sequence":"additional","affiliation":[{"name":"Chemical Engineering Research Center Tianjin Key Laboratory of Membrane Science and Desalination Technology Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) State Key Laboratory of Chemical Engineering and Low\u2010Carbon Technology (Tianjin University) School of Chemical Engineering and Technology Tianjin University Tianjin China"},{"name":"Haihe Laboratory of Sustainable Chemical Transformations  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhihua","family":"Qiao","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Technology Tiangong University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9139-9835","authenticated-orcid":false,"given":"Jingwei","family":"Hou","sequence":"additional","affiliation":[{"name":"Nanomaterials Centre School of Chemical Engineering The University of Queensland  St Lucia QLD Australia"},{"name":"ARC Centre of Excellence for Green Electrochemical Transformation of Carbon Dioxide  Brisbane Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Anthony K.","family":"Cheetham","sequence":"additional","affiliation":[{"name":"Materials Research Laboratory University of California  Santa Barbara California USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhi","family":"Wang","sequence":"additional","affiliation":[{"name":"Chemical Engineering Research Center Tianjin Key Laboratory of Membrane Science and Desalination Technology Collaborative Innovation 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