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Deep eutectic electrolytes (DEEs) offer potential solutions, yet their practical application is limited by their unsatisfactory interfacial compatibility. This study develops a non\u2010flammable quasi\u2010solid electrolyte for LMBs, via incorporating a novel 3,3\u2032\u2010[oxybis(2,1\u2010ethanediyloxy)]bispropanenitrile (OCN)\u2010based DEE into a poly(butyl acrylate) (PBA) matrix, denoted as OCN\u2010PBA. By integrating both cyano and ether functional groups, the designed OCN molecule enables dual stabilization of both the cathode and anode interfaces, as the cyano group enhances oxidation stability while the ether chains improve lithium compatibility. OCN\u2010PBA possesses a unique aggregated solvation structure, which results in a high ionic conductivity (2.0 \u00d7 10\n                    <jats:sup>\u22124<\/jats:sup>\n                    S cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), a Li\n                    <jats:sup>+<\/jats:sup>\n                    transference number (0.66), and a wide electrochemical window (5.0\u00a0V). Consequently, Li|OCN\u2010PBA|Li symmetric cell delivers stable plating\/stripping over 1500 h, and Li|OCN\u2010PBA|LiFePO\n                    <jats:sub>4<\/jats:sub>\n                    cell demonstrates over 2000 stable cycles. Moreover, the OCN\u2010PBA enables excellent cyclic stability in high\u2010voltage Li|LiNi\n                    <jats:sub>0.8<\/jats:sub>\n                    Co\n                    <jats:sub>0.1<\/jats:sub>\n                    Mn\n                    <jats:sub>0.1<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    and Li|LiCoO\n                    <jats:sub>2<\/jats:sub>\n                    cells. This work proposes a novel electrolyte design strategy, providing a feasible approach for developing practical high\u2010performance LMBs with improved safety.\n                  <\/jats:p>","DOI":"10.1002\/smll.202513016","type":"journal-article","created":{"date-parts":[[2026,2,7]],"date-time":"2026-02-07T17:00:51Z","timestamp":1770483651000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cyano\u2010Ether Bifunctional Deep Eutectic Electrolytes for Stable Quasi\u2010Solid Lithium Metal Batteries"],"prefix":"10.1002","volume":"22","author":[{"given":"Nannan","family":"Geng","sequence":"first","affiliation":[{"name":"Guangxi Key Laboratory of Processing for Non\u2010ferrous Metals and Featured Materials MOE Key Laboratory of New Processing Technology for Non\u2010ferrous Metals and Materials School of Resources Environment and Materials Guangxi University  Nanning China"}]},{"given":"Chenkai","family":"Lu","sequence":"additional","affiliation":[{"name":"Future Technology School Shenzhen Technology University  Shenzhen China"}]},{"given":"Jiong","family":"Zheng","sequence":"additional","affiliation":[{"name":"Future Technology School Shenzhen Technology University  Shenzhen China"}]},{"given":"Ziqi","family":"Cai","sequence":"additional","affiliation":[{"name":"Future Technology School Shenzhen Technology University  Shenzhen China"}]},{"given":"Jiachen","family":"Wan","sequence":"additional","affiliation":[{"name":"Future Technology School Shenzhen Technology University  Shenzhen China"}]},{"given":"Guowei","family":"Geng","sequence":"additional","affiliation":[{"name":"Guangxi Key Laboratory of Processing for Non\u2010ferrous Metals and Featured Materials MOE Key Laboratory of New Processing Technology for Non\u2010ferrous Metals and Materials School of Resources Environment and Materials Guangxi University  Nanning China"}]},{"given":"Tao","family":"Yang","sequence":"additional","affiliation":[{"name":"Future Technology School Shenzhen Technology University  Shenzhen China"}]},{"given":"Guobin","family":"Zhang","sequence":"additional","affiliation":[{"name":"Future Technology School Shenzhen Technology University  Shenzhen China"}]},{"given":"Yin","family":"Cui","sequence":"additional","affiliation":[{"name":"Future Technology School Shenzhen Technology University  Shenzhen China"}]},{"given":"E. 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