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Herein, we develop a quasi-single-ion-conducting polymer electrolyte by embedding a crown ether-functionalized covalent organic framework (COF) into a fluorinated polymer matrix. Imine (C=N) linkages in the COF and polar fluorinated polymer domains cooperatively immobilize TFSI\u2212 via electrostatic adsorption and pore-defined confinement, while the imine sites and crown ether oxygens dynamically decouple Li+ from its counter-anion and provide exchangeable coordination nodes for rapid interlayer migration along ordered COF channels. As a result, the electrolyte delivers a high ionic conductivity of 1.15\u00a0\u00d7\u00a010\u22123\u00a0S cm\u22121 with a high Li+ transference number of 0.91, establishing a continuous Li+-preferential transport network that homogenizes ion flux, promotes the formation of thin and compact interphases, and stabilizes Li anodes and high-voltage cathodes. This crown ether\u2013COF design establishes a broadly applicable design paradigm for decoupling ion transport and interfacial chemistry, paving the way toward next-generation long-lifetime Li metal batteries.<\/jats:p>","DOI":"10.1093\/nsr\/nwag098","type":"journal-article","created":{"date-parts":[[2026,2,12]],"date-time":"2026-02-12T12:52:13Z","timestamp":1770900733000},"source":"Crossref","is-referenced-by-count":5,"title":["Crown-ether-programmed covalent organic framework nanochannels enable quasi-single-ion conductivity for solid-state lithium metal batteries"],"prefix":"10.1093","volume":"13","author":[{"given":"Yihang","family":"Nie","sequence":"first","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Optical Information Materials and Technology, South China Academy of Advanced Optoelectronics, International Academy of Optoelectronics at Zhaoqing, South China Normal University , Guangzhou 510006 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