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Herein, we unravel cross\u2010scale mechanically interlocked poly(lactic acid) (CSMI\u2010PLA) nanofibrous membranes fabricated via primary hydrogen bonding through polydopamine adhesion and secondary coordinate bonding via heterogeneous metal\u2010organic frameworks entanglement. This hierarchically interlocked interface design establishes robust connectivity across dimensional scales, endowing CSMI\u2010PLA with exceptional mechanical resilience and long\u2010term sensing\u2010protective durability. Remarkably, the CSMI\u2010PLA membranes simultaneously achieve &gt;99.45% removal of PM\n                    <jats:sub>0.3<\/jats:sub>\n                    with an ultralow pressure drop of 120\u00a0Pa, a record sulfur dioxide\/nitrogen (SO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    ) selectivity of 37000, and a substantial SO\n                    <jats:sub>2<\/jats:sub>\n                    uptake of 10.6\u00a0mmol\u00b7g\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    . Moreover, the CSMI\u2010PLA membranes retain high functional integrity under multicomponent conditions while offering intrisical electroactivity that enables passive intelligent sensing. This work establishes a generalizable platform for engendering sensing\u2010protective nanofibers, with promising implications for molecularly gated sieving and biodegradable self\u2010adaptive wearables.\n                  <\/jats:p>","DOI":"10.1002\/adma.74439","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T18:15:30Z","timestamp":1785867330000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Record Selectivity of SO\n                    <sub>2<\/sub>\n                    by Molecularly Gated Sieving Membranes Having Cross\u2010Scale Mechanically Interlocked Nanofibers"],"prefix":"10.1002","volume":"38","author":[{"given":"Shao\u2010Zhen","family":"Wang","sequence":"first","affiliation":[{"name":"School of Safety Engineering China University of Mining and Technology  Xuzhou P. R. 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