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Chemical prelithiation is widely used to compensate for irreversible lithium loss and improve the initial Coulombic efficiency of silicon\u2010based anodes; however, conventional lithium\u2013arene complexes capable of directly lithiating silicon often suffer from poor chemical stability and limited practical applicability. Here, we employ a chemically stable lithium\u2013biphenyl complex in tetrahydrofuran (Li\u2013BP\/THF) that is thermodynamically incapable of directly lithiating silicon. Instead, lithium is preferentially accommodated within the surrounding hard carbon (HC) framework, while SEI pre\u2010formation also contributes to compensating initial lithium loss in silicon\u2010based composite anodes. This carbon\u2010mediated lithiation process simultaneously induces the formation of a uniform inorganic\u2010rich solid electrolyte interphase, which stabilizes interfacial reactions during subsequent cycling. Furthermore, the efficiency of the prelithiation process is governed by the structural characteristics of the HC framework, which can be systematically tuned through controlled heat treatment. Overall, this work establishes Li\u2013BP\/THF\u2010mediated carbon\u2010assisted chemical prelithiation as a chemically stable strategy for minimizing initial lithium loss while enhancing interfacial stability in silicon\u2010based composite anodes.<\/jats:p>","DOI":"10.1002\/smll.74926","type":"journal-article","created":{"date-parts":[[2026,7,30]],"date-time":"2026-07-30T07:42:31Z","timestamp":1785397351000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Carbon\u2010Mediated Lithium Hosting for Prelithiation of Silicon\u2013Hard Carbon Anodes Without Direct Silicon Lithiation"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-4907-1711","authenticated-orcid":false,"given":"Hyerin","family":"Jeon","sequence":"first","affiliation":[{"name":"Department of Chemistry and Chemical Engineering Inha University  Incheon Republic of 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