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However, increasing sulfur loading inevitably deteriorates charge\u2010transport efficiency and slows electrochemical reaction kinetics, leading to pronounced degradation in rate capability and cycling stability. To address these critical challenges, a biomimetic strategy is adopted to engineer gradient\u2010porous nitrogen\u2010doped carbon nanomaterials (Bio\u2010N\u2010CNTs) with radially graded pore architectures, enabling their use as highly effective sulfur host materials. In situ Raman spectroscopy and DFT reveal that such unique structures facilitate efficient mass transport, ion diffusion, sulfur conversion, and high sulfur loading simultaneously, as well as enable gradient confinement catalytic conversion of LiPSs. As a result, the Bio\u2010N\u2010CNT\/S cathode exhibits a capacity decay rate of only 0.178% after 100 cycles at a 0.1 C rate. Even under high sulfur loading conditions of 8.6\u00a0mg cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , this cathode material maintains 71% capacity retention after 100 cycles. Additionally, a sustainable \u201cprecipitation\u2010enrichment\u2010reduction\u2010regeneration\u201d silver recovery strategy with a 93% recovery rate, enhancing economic feasibility. This work demonstrates an innovative, scalable, and sustainable biomimetic Bio\u2010N\u2010CNT host for practical Li\u2013S batteries.\n                  <\/jats:p>","DOI":"10.1002\/anie.5836599","type":"journal-article","created":{"date-parts":[[2026,4,13]],"date-time":"2026-04-13T12:27:37Z","timestamp":1776083257000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Biomimetic Gradient\u2010Porous Carbon Enables Sustainable High\u2010Loading Lithium\u2013Sulfur Batteries by Regulating Polysulfide Chemistry"],"prefix":"10.1002","volume":"65","author":[{"given":"Zihai","family":"Cheng","sequence":"first","affiliation":[{"name":"Division of Energy Conversion &amp; Storage, Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, CAS Key Laboratory of Mechanical Behavior and Design of Materials (LMBD), School of Engineering Science University of Science and 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Environmental Science and Engineering University of Science and Technology of China  Hefei Anhui China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7494-1469","authenticated-orcid":false,"given":"Haibo","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Anhui University  Hefei Anhui China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wujun","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Environmental Technology Department of Environmental Science and Engineering University of Science and Technology of China  Hefei Anhui China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2580-928X","authenticated-orcid":false,"given":"Li\u2010Feng","family":"Chen","sequence":"additional","affiliation":[{"name":"Division of Energy Conversion &amp; Storage, Hefei National Research 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