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Herein, a new sealing method is introduced by combining a fluorinated polymer and reactive ion plasma treatment to physically tune the permeation of the polycrystalline zeolitic imidazolate framework\u20108 (ZIF\u20108) membranes. In particular, the sealing technique is applied to the ZIF\u20108 membrane hybridized with graphene nanoribbon with an intrinsic aperture size of 3.4 \u212b, and the sealing method can be easily tuned depending on the target gas pairs. First, the ultrathin perfluoropolyether (PFPE) layer, formed <jats:italic>via<\/jats:italic> dip\u2010coating, effectively blocks the permeation of large molecules through the non\u2010selective grain boundaries, resulting in the H<jats:sub>2<\/jats:sub> permeance of 1.3 \u00d7 10<jats:sup>\u22126<\/jats:sup> mol\u00a0m<jats:sup>\u22122<\/jats:sup>\u00b7Pa\u00b7s and 209 of the ideal H<jats:sub>2<\/jats:sub>\/N<jats:sub>2<\/jats:sub> selectivity. Second, methane permeation can be further hindered by additional reactive ion plasma treatment, which enhances the fluorination of the sealing layer, resulting in 1218 of the ideal H<jats:sub>2<\/jats:sub>\/CH<jats:sub>4<\/jats:sub> selectivity. Due to the physical confinement with graphene nanoribbon and thin sealing layer, the membrane is highly selective and permeable for hydrogen, far surpassing the performance of previous MOF\u2010type membranes. Molecular dynamics simulations reveal MOF membranes' critical grain boundary gap degrading selectivity.<\/jats:p>","DOI":"10.1002\/smll.202501590","type":"journal-article","created":{"date-parts":[[2025,7,13]],"date-time":"2025-07-13T12:09:57Z","timestamp":1752408597000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Gas\u2010Specific and Tunable Hydrogen\u2010Selective ZIF Membrane through Combined Physical Confinement and Sealing Techniques"],"prefix":"10.1002","volume":"21","author":[{"given":"Eunji","family":"Choi","sequence":"first","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Yonsei University  Yonsei\u2010ro 50, Seodaemun\u2010gu Seoul 03722 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Seungho","family":"Yu","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering Konkuk University  Seoul 05029 Republic of 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