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However, issues such as irreversible lithium loss caused by uneven solid electrolyte interphase (SEI) on anode during the charging\/discharging process, along with severe volume changes leading to structural instability, are key factors limiting their lifespan far below practical application. Herein, a sphere\u2212sheet hetero\u2212interlayer (2DLP\u2212PASF) is designed, which adapts to volume changes and exhibits Li\n                    <jats:sup>+<\/jats:sup>\n                    selectivity. The interlayer is fabricated by electrophoretic deposition of \u2212SO\n                    <jats:sub>3<\/jats:sub>\n                    Li rich elastic ionomer emulsion (PASF) particles and laponite nanosheets (2DLP) onto a copper current collector. The elastic PASF particles support 2DLP to form a dispersed stress\u2212buffering structure, which can accommodate volume changes during the charging\/discharging process and suppress dendrite growth. Furthermore, rich \u2212SO\n                    <jats:sub>3<\/jats:sub>\n                    Li in densely packed PASF shells between 2DLP repel anions electrostatically through the Donnan effect, which facilitates efficient Li\n                    <jats:sup>+<\/jats:sup>\n                    transport and flux homogenization, thereby inhibiting the polysulfide shuttle. Additionally, \u2212C\u2261N and \u2212CF\n                    <jats:sub>3<\/jats:sub>\n                    in PASF cores transform into a stable, Li\n                    <jats:sub>3<\/jats:sub>\n                    N\/LiF\u2212rich secondary SEI on anode, which in turn synergizes with the tough 2DLP\u2212PASF to further stabilize lithium deposition. As a result, the AFLSB assembled with 2DLP\u2212PASF modified copper current collector and Li\n                    <jats:sub>2<\/jats:sub>\n                    S cathode demonstrated significantly improved comprehensive electrochemical performance.\n                  <\/jats:p>","DOI":"10.1002\/anie.2370748","type":"journal-article","created":{"date-parts":[[2026,9,12]],"date-time":"2026-09-12T17:12:01Z","timestamp":1789233121000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Sphere\u2212Sheet Hetero\u2212Interlayer With Mechanoadaptivity and Li\n                    <sup>+<\/sup>\n                    Selectivity for High Performance Anode Free Lithium Sulfur Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Chao","family":"Ding","sequence":"first","affiliation":[{"name":"Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yifan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiacheng","family":"Lin","sequence":"additional","affiliation":[{"name":"Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fangrong","family":"Xiao","sequence":"additional","affiliation":[{"name":"Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenxu","family":"Zheng","sequence":"additional","affiliation":[{"name":"Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4425-6636","authenticated-orcid":false,"given":"Wenqiang","family":"Wang","sequence":"additional","affiliation":[{"name":"Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and Engineering East China University of 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