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In this work, we propose iodine-induced charge transfer of a covalent organic framework (COF) as an effective strategy to achieve fast ion transport and a stable SSE\/Li interface. First, the electron-deficient COF skeleton in the I2\/COF charge-transfer complex anchors TFSI- anions through enhanced electrostatic interactions, thereby promoting the dissociation of lithium salt to release free Li+. Second, the electron deficiency of COF strengthens its dipole\u2013dipole interactions with PEO, leading to suppressed PEO crystallization and enhanced COF\/PEO compatibility. Third, the electron-deficient COF tailors the Li+ coordination environment via weakening the affinity of PEO and COF toward Li+. Consequently, the I2\/COF charge-transfer complex accelerates Li+ transport kinetics in PEO-based composite SSEs. Furthermore, the confinement effect of COF toward I2 via charge transfer effectively inhibits the aggressive lithium anode corrosion by I2, resulting in the controlled growth of a stable, robust, and conductive solid electrolyte interface (SEI) rich in LiF and LiI. Thus, the I2\/COF charge-transfer complex enables excellent rate capability and cycling stability of the resulting COF\/PEO-based composite SSE, maintaining a capacity retention of 88.58% after 1000 cycles at 2 C. This work offers a promising strategy for designing COF\/PEO-based composite SSEs for next-generation all-solid-state lithium metal batteries.<\/jats:p>","DOI":"10.1021\/acsami.6c15793","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T17:06:49Z","timestamp":1791479209000},"page":"56182-56191","source":"Crossref","is-referenced-by-count":0,"title":["Enabling Efficient Ion Transport and Stable Interfaces of PEO-Based Solid Electrolytes via an I2\/COF Charge-Transfer Complex"],"prefix":"10.1021","volume":"18","author":[{"given":"Jing","family":"Li","sequence":"first","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaping","family":"Sun","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing","family":"Li","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9016-832X","authenticated-orcid":true,"given":"Cheng","family":"Lian","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]},{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4744-9692","authenticated-orcid":true,"given":"Haiping","family":"Su","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1699-3089","authenticated-orcid":true,"given":"Jingkun","family":"Li","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5682-2295","authenticated-orcid":true,"given":"Honglai","family":"Liu","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]},{"name":"East China University of Science and Technology , , ,","place":["Shanghai, PR China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,6]]},"reference":[{"issue":"39","key":"2026102609075255200_cit1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202508281","article-title":"Manipulating Competitive Li+ Coordination of F-Rich Polymer and High Flash Point Glyme Electrolyte Enabling High Rate and Intrinsically Safe Quasi-Solid-State Li Metal Batteries","volume":"64","author":"Zhang","year":"2025","journal-title":"Angew. 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