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However, dense structures hinder proton transport and cause progressive deformation during cell operation, reducing overall performance. In this study, sub\u201025 nm ultrathin PFSA membranes are demonstrated by harnessing engineered microdefects as size\u2010exclusive pores, promoting proton transport while maintaining structural integrity. To achieve this, only 14 molecularly thin PFSA Langmuir monolayers are stacked with adjusted packing density, and proton\u2010conducting pathways are sufficiently established via pre\u2010swelling. Unlike conventional strategies for robust dense membranes, this approach suppresses deformation of the channel morphology during cell operation, with higher ion selectivity than Nafion 211. Finally, the optimized ultrathin membrane exhibits superior cyclic and rate performance compared to the commercial membrane, delivering \u224876% energy efficiency and long\u2010term stability at 200\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    without capacity decay.\n                  <\/jats:p>","DOI":"10.1002\/smll.202500505","type":"journal-article","created":{"date-parts":[[2025,6,13]],"date-time":"2025-06-13T06:45:11Z","timestamp":1749797111000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Engineered Microdefects in Nano\u2010Membranes for Enhanced Ion Selectivity and Membrane Durability in Vanadium Redox Flow Batteries"],"prefix":"10.1002","volume":"21","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5294-1844","authenticated-orcid":false,"given":"Jongmin Q.","family":"Kim","sequence":"first","affiliation":[{"name":"Interface Materials and Chemical 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