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Although polyoxometalates (POMs) are promising proton conductors, their practical application is hindered by poor processability, susceptibility to leaching, and difficulty in forming continuous proton conduction pathways within polymers. Herein, a new photocurable polyoxometalate (POM)\u2010organic membrane (PAPOM\u2010AMPS) is synthesized via ultrafast UV\u2010initiated copolymerization of an acrylamide\u2010functionalized arsenomolybdate cluster (APOM), 2\u2010acrylamido\u20102\u2010methylpropanesulfonic acid (AMPS), and acrylic acid (AA). This molecular\u2010level design ingeniously constructs hierarchical proton transport channels: the covalently immobilized APOM clusters serve as long\u2010range highways, while sulfonic (\u2013SO\n                    <jats:sub>3<\/jats:sub>\n                    H) and carboxylic (\u2013COOH) acid groups synergize with water molecules to facilitate efficient proton dissociation and dynamic short\u2010range hopping. The membrane exhibits an exceptional proton conductivity of 0.417 S\u00b7cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 80\u00b0C and 100% RH, surpassing Nafion 117. With confined ionic domains (\u223c2.27 nm), it achieves ultrahigh proton\/vanadium selectivity (18.1 \u00d7 10\n                    <jats:sup>4<\/jats:sup>\n                    S\u00b7min\u00b7cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    ), 4.6 times that of Nafion 117. When configured into a sandwich\u2010structured membrane for vanadium flow batteries (VFBs), it delivers outstanding performance, including 98.2% coulombic efficiency, 86.7% energy efficiency, and exceptional cycling stability (0.12% capacity decay per cycle at 120 mA\u00b7cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    ). This work provides a groundbreaking strategy for next\u2010generation high\u2010performance proton\u2010conductive membranes.\n                  <\/jats:p>","DOI":"10.1002\/anie.3224554","type":"journal-article","created":{"date-parts":[[2026,7,3]],"date-time":"2026-07-03T17:04:22Z","timestamp":1783098262000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["A Photocurable Covalent Polyoxometalates\u2010Membrane With Hierarchical Proton Conduction Pathways for High\u2010Performance Vanadium Flow Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Xin","family":"Mu","sequence":"first","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of Chemistry Northeast Normal University  Changchun P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianlu","family":"Li","sequence":"additional","affiliation":[{"name":"China Huaneng International Engineering &amp; Technology Co. Ltd.  Xiong'an Hebei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhen","family":"Sun","sequence":"additional","affiliation":[{"name":"China Huaneng International Engineering &amp; Technology Co. Ltd.  Xiong'an Hebei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhongling","family":"Lang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of Chemistry Northeast Normal University  Changchun P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5952-5077","authenticated-orcid":false,"given":"Huaqiao","family":"Tan","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of Chemistry Northeast Normal University  Changchun P. R. 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