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Here, we present a metal\u2013organic framework (MOF) channel membrane that combines two complementary ion\u2010conduction motifs: carboxyl groups from UiO\u201066\u2010COOH and carboxybenzo\u201015\u2010crown\u20105 (15C5\u2010COOH), assembled in a one\u2010step coordination strategy. This hybrid architecture recapitulates essential NaK channel functions, offering both ultrahigh ion selectivity and controllable gating. The membrane enables highly selective conduction of monovalent cations while effectively excluding Mg\n                    <jats:sup>2+<\/jats:sup>\n                    , yielding M\n                    <jats:sup>+<\/jats:sup>\n                    \/Mg\n                    <jats:sup>2+<\/jats:sup>\n                    selectivity above 10\n                    <jats:sup>2<\/jats:sup>\n                    . Under mixed\u2010ion conditions, it achieves unprecedented Na\u207a\/K\u207a selectivity exceeding 10\n                    <jats:sup>3<\/jats:sup>\n                    , far surpassing reported artificial ion channels. Remarkably, Mg\n                    <jats:sup>2+<\/jats:sup>\n                    ions dynamically gate Na\u207a and K\u207a transport with sustainable on\u2013off ratios around 30. These outstanding performances arise from the synergistic interplay of crown ether and carboxyl groups confined within subnanometer MOF pores. This work establishes a versatile strategy for designing multifunctional artificial ion channels, opening avenues toward advanced ionic devices for artificial cells and biomedical technologies.\n                  <\/jats:p>","DOI":"10.1002\/anie.202521527","type":"journal-article","created":{"date-parts":[[2026,1,10]],"date-time":"2026-01-10T14:04:51Z","timestamp":1768053891000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Biomimetic NaK Channel Membrane Enabled by a Crown Ether\u2010Coordinated Metal\u2013Organic Framework"],"prefix":"10.1002","volume":"65","author":[{"given":"Chen","family":"Zhao","sequence":"first","affiliation":[{"name":"Department of Chemical and Environmental Engineering RMIT University  Melbourne VIC 3000 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Na","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemical and Environmental 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