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Inspired by the \u201cvein-mesophyll\u201d structure of Cinnamomum camphora leaves, we constructed a mechanically robust dual-path ion-conductive biomimetic interphase (PVLN) via filler alignment and a localized high-concentration electrolyte (LHCE) strategy to stabilize the LATP\/Li interface. In the PVLN interlayer, the PVDF-HFP-based LHCE confines DMSO and regulates the local solvent environment, while the well-aligned LATP particles on the PAN substrate provide abundant Li+ coordination and transport sites. This coupled structure decouples ion pairing from ion conduction, facilitates Li+ desolvation and migration, and promotes the formation of continuous Li+ transport pathways. More importantly, neutron powder diffraction analysis elucidated the stable Ti4+ of the PVLN@LATP during cycling, which significantly indicates the PVLN interlayer can reduce the detrimental reduction reactions at the LATP\/Li interface, which is rarely reported. As a result, the PVLN@LATP composite exhibits an ionic conductivity of 5.1 \u00d7 10\u20134 S cm\u20131 and a wide electrochemical stability window of up to 4.85 V. Leveraging these synergistic effects, the Li|PVLN@LATP|Li symmetric cell tested at room temperature achieves stable cycling for over 3000 h, demonstrating excellent interfacial compatibility. This biomimetic composite strategy provides insights and avenues for designing multiphase structures in solid-state batteries.<\/jats:p>","DOI":"10.1021\/acsami.6c08058","type":"journal-article","created":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T07:27:58Z","timestamp":1788247678000},"page":"47578-47590","source":"Crossref","is-referenced-by-count":0,"title":["A Mechnically Robust Dual-Path Ion-Conductive Biomimetic Interfacial Layer Engineered via Solvation Structure for Ultrastable LATP Solid-State Batteries"],"prefix":"10.1021","volume":"18","author":[{"given":"Haiting","family":"Shi","sequence":"first","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiale","family":"Song","sequence":"additional","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junhao","family":"Wang","sequence":"additional","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]},{"name":"Shanghai Synchrotron Radiation Facility, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201204"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingjie","family":"Dong","sequence":"additional","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rongrong","family":"Yu","sequence":"additional","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xianyan","family":"Wu","sequence":"additional","affiliation":[{"name":"Jiaxing University , , ,","place":["Jiaxing, China, 314001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Amna","family":"Siddique","sequence":"additional","affiliation":[{"name":"National Textile University , , Sheikhupura Road , ,","place":["Faisalabad, Pakistan, 37610"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juan","family":"Zhou","sequence":"additional","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Feng","family":"Tian","sequence":"additional","affiliation":[{"name":"Shanghai Synchrotron Radiation Facility, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201204"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuanbin","family":"Yu","sequence":"additional","affiliation":[{"name":"Yangzhou University , , , ,","place":["Yangzhou, Jiangsu, China, 225127"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7015-3457","authenticated-orcid":true,"given":"Yong","family":"Liu","sequence":"additional","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8067-5344","authenticated-orcid":true,"given":"Zhiwei","family":"Xu","sequence":"additional","affiliation":[{"name":"Tiangong University , , ,","place":["Tianjin, China, 300387"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,26]]},"reference":[{"issue":"49","key":"2026091612071361900_cit1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202207232","article-title":"Electro\u2013Chemo\u2013Mechanical Failure of Solid Electrolytes Induced by Growth of Internal Lithium Filaments","volume":"34","author":"Xu","year":"2022","journal-title":"Adv. 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