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Conventional polymer electrolytes with electronegative groups strongly adsorb high\u2010valent nickel, accelerating cathode decomposition and oxygen release. Here, we develop a deep\u2010eutectic polymer electrolyte (p\u2010DEPE) via in situ copolymerization of cyanoacrylate and butyl acrylate within a LiTFSI\/LiDFOB dual\u2010salt network to reshape the interfacial chemistry. This design creates an intermolecular hydrogen\u2010bonding matrix that establishes a competitive coordination environment at the cathode interface, effectively weakening Ni\n                    <jats:sup>4+<\/jats:sup>\n                    adsorption on electronegative sites. The suppression of high\u2010value Ni inhibits the growth of a high\u2010resistance cathode\u2013electrolyte interphase and retards the detrimental phase transition from a layered to a rock\u2010salt structure. Furthermore, the locally confined interaction between the cyano\u2010group and the cathode surface at high states of charge minimizes parasitic chemical reactions with lattice oxygen, thereby substantially reducing oxygen release. Consequently, 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                    cells with p\u2010DEPE deliver outstanding high\u2010rate performance, cycling over 200 cycles at 2 C at room temperature and at 3 C at 70\u00b0C. Moreover, a 4.5\u00a0V high\u2010loading Li||NCM811 pouch cell retains 97.3% of its initial capacity after 100 cycles. This work demonstrates a scalable polymer electrolyte strategy for high\u2010energy\u2010density lithium metal batteries.\n                  <\/jats:p>","DOI":"10.1002\/advs.75883","type":"journal-article","created":{"date-parts":[[2026,5,30]],"date-time":"2026-05-30T09:49:16Z","timestamp":1780134556000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Deep Eutectic Polymer Electrolyte with Competitive Hydrogen\u2010Bonding Coordination for High\u2010Voltage Nickel\u2010rich Lithium Metal Batteries"],"prefix":"10.1002","volume":"13","author":[{"given":"Yuxin","family":"Fan","sequence":"first","affiliation":[{"name":"State Key Laboratory of Electronic Thin Films and Integrated Devices University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Miao","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of 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