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Herein, we propose an atomic level precise pore engineering strategy that integrates pore confinement with surface polarization in a metal\u2010organic framework (MOF) CAU\u201010\u2010PyDC. The electron\u2010withdrawing effect of the pyridinic nitrogen atoms induces a localized positively charged microenvironment, which strongly anchors anions, promotes NaTFSI dissociation and establishes ion\u2010decoupled transport pathways with low energy barriers. Simultaneously, the optimized pore size offers a low\u2010energy\u2010barrier pathway for efficient Na\n                    <jats:sup>+<\/jats:sup>\n                    migration. Importantly, CAU\u201010\u2010PyDC synergistically promoted polymer electrolyte (PyDC\u2010MSPE) induces the formation of stable, inorganic\u2010rich SEI and CEI layers, effectively suppressing dendrite growth and interfacial side reactions. The PyDC\u2010MSPE electrolyte demonstrates a high ionic conductivity of 3.37\u00d710\n                    <jats:sup>\u22124<\/jats:sup>\n                    S cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    and a Na\n                    <jats:sup>+<\/jats:sup>\n                    transference number of 0.75. Na|PyDC\u2010MSPE|Na\n                    <jats:sub>3<\/jats:sub>\n                    V\n                    <jats:sub>2<\/jats:sub>\n                    (PO\n                    <jats:sub>4<\/jats:sub>\n                    )\n                    <jats:sub>3<\/jats:sub>\n                    ASSP\u2010SMB maintains a specific capacity of 111.2 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    after 1000 cycles at 2C. The corresponding pouch cell achieves an energy density of 325.7\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    , with high\u2010capacity retention of 87.7% after 100 cycles. This study unveils a novel mechanism where pore confinement synergizes surface polarization to regulate ion transport, offering an effective approach to addressing sodium salt dissociation and ion transport challenges in ASSP\u2010SMBs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202525120","type":"journal-article","created":{"date-parts":[[2026,2,15]],"date-time":"2026-02-15T08:38:06Z","timestamp":1771144686000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Anion\u2010Immobilized Polar Nanochannels in Metal\u2010Organic Frameworks Enable Ion\u2010Decoupled Transport for High\u2010Performance Solid\u2010State Sodium Batteries"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9883-8888","authenticated-orcid":false,"given":"Tianlin","family":"Li","sequence":"first","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5548-3367","authenticated-orcid":false,"given":"Danyang","family":"Zhao","sequence":"additional","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"},{"name":"Jiangsu Province Engineering Laboratory of High\u2010Efficient Energy Storage Technology and Equipment School of Materials Science and Physics China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Meiyu","family":"Shi","sequence":"additional","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hanqing","family":"Jiao","sequence":"additional","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuai","family":"Zheng","sequence":"additional","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qing","family":"Yin","sequence":"additional","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"},{"name":"Jiangsu Province Engineering Laboratory of High\u2010Efficient Energy Storage Technology and Equipment School of Materials Science and Physics China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiqiu","family":"Qi","sequence":"additional","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"},{"name":"Jiangsu Province Engineering Laboratory of High\u2010Efficient Energy Storage Technology and Equipment School of Materials Science and Physics China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yong\u2010Zhi","family":"Li","sequence":"additional","affiliation":[{"name":"China University of Mining and Technology  Xuzhou 221116 P R China"},{"name":"Jiangsu Province Engineering Laboratory of High\u2010Efficient Energy Storage Technology and Equipment School of Materials Science and Physics China University of Mining and Technology  Xuzhou 221116 P R China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2874-9326","authenticated-orcid":false,"given":"Lei","family":"Hou","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry &amp; Materials Science Northwest University  Xi'an 710127 P.R. 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