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However, achieving high thermal conductivity alongside strong adhesion and low viscosity remains a fundamental challenge due to conflicting material requirements. Herein, a molecularly engineered thermally conductive adhesive is reported that uniquely and simultaneously overcomes these trade\u2010offs by integrating amino\u2010 and phenylboronic acid\u2010functionalized hyperbranched polysiloxane into a polydimethylsiloxane matrix filled with multi\u2010scale aluminum fillers. A coupled dynamic\u2010covalent network originating from the hyperbranched polysiloxane enhances both bulk and interfacial dissipation through reversible boronic\u2010ester exchange, while the multi\u2010scale aluminum architecture increases maximum packing and connectivity yet suppresses viscosity growth, enabling ultra\u2010high filler loading without sacrificing bonding. The resulting thermally conductive adhesive achieves a thermal conductivity of 6.21\u00a0W\u00a0m\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0K\n                    <jats:sup>\u22121<\/jats:sup>\n                    , an adhesion strength of 5.13\u00a0MPa, and a low viscosity of 253.0\u00a0Pa\u00a0s. Device\u2010level validation confirms its excellent dispensability, ability to lower operational temperature and relieve thermomechanical stress, thereby establishing a distinct design paradigm that links molecular structure, filler architecture, and thermo\u2010mechanical reliability in one coherent framework.\n                  <\/jats:p>","DOI":"10.1002\/smll.202510272","type":"journal-article","created":{"date-parts":[[2025,11,11]],"date-time":"2025-11-11T10:16:09Z","timestamp":1762856169000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Breaking the Thermal Conductivity\u2013Adhesion\u2013Viscosity Trade\u2010off in Thermally Conductive Adhesive via Hyperbranched Networks and Multi\u2010Scale Fillers"],"prefix":"10.1002","volume":"21","author":[{"given":"Yuanyuan","family":"Xiao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Materials for Integrated Circuits Shenzhen Institute of Advanced Electronic Materials Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences  Shenzhen 518055 China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yabiao","family":"Ma","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Materials for Integrated Circuits Shenzhen Institute of Advanced Electronic Materials Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences  Shenzhen 518055 China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shujun","family":"Cai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Materials for Integrated Circuits Shenzhen Institute of Advanced Electronic Materials Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences  Shenzhen 518055 China"},{"name":"Nano Science and Technology 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1389-8484","authenticated-orcid":false,"given":"Xiaoliang","family":"Zeng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Materials for Integrated Circuits Shenzhen Institute of Advanced Electronic Materials Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences  Shenzhen 518055 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