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Here we report a layer\u2010by\u2010layer MXene\/PFSA membrane architecture in which MXene nanosheets are integrated into PFSA coating layers to create MXene\u2010regulated nanointerfaces that decouple proton conductivity from gas and ion permeation. The lamellar MXene framework introduces tortuous transport pathways and selectively perturbs PFSA hydrophilic domain organization while preserving continuous proton\u2010conducting networks through interfacial hydrogen bonds. As a result, the optimized membrane exhibits simultaneously enhanced H\n                    <jats:sup>+<\/jats:sup>\n                    \/H\n                    <jats:sub>2<\/jats:sub>\n                    and H\n                    <jats:sup>+<\/jats:sup>\n                    \/VO\n                    <jats:sup>2+<\/jats:sup>\n                    selectivity, achieving up to 43.0% lower hydrogen permeability and 37.5% reduced vanadium ion diffusion compared to pristine PFSA, without sacrificing proton conductivity. It exhibits stable long\u2010term operation in PEMWE with lower hydrogen and retains 67.0% capacity in VRFB over 470 cycles, outperforming pristine PFSA more than 40% of capacity retention. Small\u2010 and wide\u2010angle X\u2010ray scattering reveal MXene\u2010induced disordering and expansion of large\u2010scale hydrophilic domains, while density functional theory (DFT) calculations reveal that the MXene\/PFSA interface selectively increases transport energy barriers for hydrogen and vanadium ions while preserving low barriers for proton migration. These results validate a versatile interfacial strategy toward overcoming selectivity limitations for both PEMWE and VRFB.\n                  <\/jats:p>","DOI":"10.1002\/advs.78270","type":"journal-article","created":{"date-parts":[[2026,10,14]],"date-time":"2026-10-14T19:41:59Z","timestamp":1792006919000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dual\u2010Functional Membranes With Interfacial MXene\/PFSA Nanoarchitectures for Low Hydrogen Permeation in Water Electrolysis and Reduced Vanadium Ion Crossover in Flow Batteries"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0077-9504","authenticated-orcid":false,"given":"Panpan","family":"Guan","sequence":"first","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingjia","family":"Jiang","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunhu","family":"Jiang","sequence":"additional","affiliation":[{"name":"Shandong Key Laboratory of Core Materials and Technologies for Hydrogen Energy and Dongyue Future Hydrogen Energy Materials Company  Zibo China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0198-0330","authenticated-orcid":false,"given":"Wei","family":"Li","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yecheng","family":"Zou","sequence":"additional","affiliation":[{"name":"Shandong Key Laboratory of Core Materials and Technologies for Hydrogen Energy and Dongyue Future Hydrogen Energy Materials Company  Zibo China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lixiao","family":"Zhang","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaifeng","family":"Long","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4777-4017","authenticated-orcid":false,"given":"Ziqi","family":"Sun","sequence":"additional","affiliation":[{"name":"School of Chemistry and Physics Queensland University of Technology  Brisbane Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ting","family":"Liao","sequence":"additional","affiliation":[{"name":"Faculty of Engineering School of Mech. Medical &amp; Process Engineering Queensland University of Technology  Brisbane Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0253-647X","authenticated-orcid":false,"given":"Hua Kun","family":"Liu","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5432-6378","authenticated-orcid":false,"given":"Ding","family":"Yuan","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0074-7633","authenticated-orcid":false,"given":"Dingsheng","family":"Wang","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3824-7693","authenticated-orcid":false,"given":"Shi Xue","family":"Dou","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2549-1400","authenticated-orcid":false,"given":"Yuhai","family":"Dou","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,14]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41893\u2010024\u201001317\u20107"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jclepro.2023.140476"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202415755"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1007\/s12274\u2010024\u20106972\u2010z"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2024.148543"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1007\/s12274\u2010024\u20106900\u20106"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1007\/s12274\u2010024\u20106460\u20105"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202402090"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202314956"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemmater.2c01445"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.6b00159"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adh1386"},{"key":"e_1_2_8_14_1","doi-asserted-by":"crossref","first-page":"16003","DOI":"10.1021\/acsnano.2c03730","article-title":"Kinetic Control of Angstrom\u2010Scale Porosity in 2D Lattices for Direct Scalable Synthesis of Atomically Thin Proton Exchange Membranes","volume":"16","author":"Moehring N. 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