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However, traditional high-loading thermal management materials suffer from an intrinsic mechanical-thermal trade-off. Herein, we propose a tough hydrogel-mediated constrained assembly strategy. By introducing carbon nanotubes (CNT) to enhance the interfacial interactions between poly(p-phenylene benzobisoxazole) (PBO) nanofibers and graphene nanosheets (GNS), a robust hydrogel intermediate is constructed. This stable intermediate unlocks the processing window for high-loading systems, allowing them to be dried into films under a 30% in-plane tensile constraint. The composite film achieves long-range orientation and extreme densification of two-dimensional (2D) nanosheets, forming a continuous multidimensional thermally conductive network via cross-scale CNT bridging. Consequently, the film exhibits a concurrent mechanical-thermal enhancement, delivering an in-plane thermal conductivity of 214 W m\u20131 K\u20131 and a tensile strength of 379.7 MPa. In practical applications, the film demonstrates outstanding bidirectional thermal management capabilities. It efficiently eliminates local hot spots in flexible electronics as a passive cooling layer and provides rapid active Joule heating to swiftly elevate the surface temperature of pouch cells. This work offers a valuable reference for next-generation flexible thermal management systems.<\/jats:p>","DOI":"10.1021\/acsami.6c17117","type":"journal-article","created":{"date-parts":[[2026,10,14]],"date-time":"2026-10-14T17:02:52Z","timestamp":1791997372000},"page":"58418-58428","source":"Crossref","is-referenced-by-count":0,"title":["Tough Hydrogel-Mediated Constrained Assembly of Multidimensional Topological Networks for Synergistic Mechanical-Thermal Enhancement"],"prefix":"10.1021","volume":"18","author":[{"given":"Guang","family":"Xiao","sequence":"first","affiliation":[{"name":"University of South China , , ,","place":["Hengyang, China, 421001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Li","sequence":"additional","affiliation":[{"name":"Henan Academy of Sciences , , ,","place":["Zhengzhou, China, 450052"]},{"name":"Xuchang University , , ,","place":["Xuchang, China, 461000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoting","family":"Niu","sequence":"additional","affiliation":[{"name":"NingboTech University , , ,","place":["Ningbo, China, 315211"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4381-2952","authenticated-orcid":true,"given":"Yagang","family":"Yao","sequence":"additional","affiliation":[{"name":"Zhejiang Sci-Tech University , , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,14]]},"reference":[{"key":"2026102915065065500_cit1","doi-asserted-by":"publisher","DOI":"10.1016\/j.pmatsci.2024.101362","article-title":"Polymer Composites with High Thermal Conductivity: Theory, Simulation, Structure and Interfacial Regulation","volume":"148","author":"Zha","year":"2025","journal-title":"Prog. 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