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However, in conventional solid\u2010state regeneration, limited solid\u2013solid contact and the premature formation of a dense conductive carbon layer hinder the effective coordination of lithium replenishment, structural defect repair, and interfacial reconstruction, thereby limiting lithium utilization efficiency and structural restoration. This paper presents a self\u2010assembled supramolecular (SAS) regeneration system spontaneously formed from trithiocyanuric acid (TMT) and lithium acetate (CH\n                    <jats:sub>3<\/jats:sub>\n                    COOLi). Through Li\u2013S coordination and hydrogen\u2010bonding interactions, the precursor self\u2010assembles into an ordered supramolecular architecture that regulates the thermal evolution of the solid\u2010state regeneration process. Unlike the independent thermal decomposition of mechanically mixed precursors in conventional solid\u2010state regeneration, the ordered supramolecular architecture regulates the reaction sequence, enabling lithium to preferentially enter the LiFePO\n                    <jats:sub>4<\/jats:sub>\n                    lattice before the formation of a dense conductive carbon layer, thereby achieving efficient lithium replenishment and structural restoration. Subsequently, an in situ generated N\/S co\u2010doped conductive carbon layer elevates interfacial conductivity of regenerated LFP. The regenerated cathode delivers 160.3 mAh g\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    (0.1 C) and 143.0 mAh g\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    (1 C), maintaining 88% capacity over 500 cycles at 1 C, while the pouch cell exhibits 81% capacity retention after 500 cycles at 0.5 C.\n                  <\/jats:p>","DOI":"10.1002\/anie.4146793","type":"journal-article","created":{"date-parts":[[2026,8,14]],"date-time":"2026-08-14T16:36:16Z","timestamp":1786725376000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Supramolecular Self\u2010Assembly Enables Controlled Lithium Replenishment Toward High\u2010Performance and Sustainable Regeneration of Spent LiFePO\n                    <sub>4<\/sub>\n                    Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Yixin","family":"Lin","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-3564-8499","authenticated-orcid":false,"given":"Tiansheng","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chaochao","family":"Gao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5220-3238","authenticated-orcid":false,"given":"Jie","family":"Xu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Harbin Institute of Technology  Harbin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawen","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zixi","family":"Lin","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guanghao","family":"Mao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weihao","family":"Gao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yixuan","family":"Tang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Sauvage Laboratory for Smart Materials School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2377-9796","authenticated-orcid":false,"given":"Jiaheng","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen)  Shenzhen China"},{"name":"Research Centre of Printed Flexible Electronics Harbin Institute of Technology (Shenzhen)  Shenzhen 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