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Conventional surface modification strategies remain fundamentally constrained by a heavy reliance on hazardous solvents, matrix curing inhibition, and structural degradation of the fillers. Herein, we report a solvent\u2010free mechanochemical copolymerization strategy that establishes an universal, non\u2010destructive interfacial engineering paradigm for diverse Group 13 and related fillers (nano\u2010Al, B\n                    <jats:sub>4<\/jats:sub>\n                    C, and ZrB\n                    <jats:sub>2<\/jats:sub>\n                    ). By directly architecting sulfur\u2010containing polymer coatings on filler surfaces, this approach elegantly exploits intrinsic Lewis acid\u2013base pairing between electron\u2010deficient metal\/metalloid sites and electron\u2010rich sulfur moieties. Mechanistically, the resulting electronic configurations and coordination chemistry are systematically elucidated via a synergistic combination of XPS, solid\u2010state\n                    <jats:sup>11<\/jats:sup>\n                    B NMR, and DFT calculations, confirming the formation of robust S\u2013Al and S\u2013B coordinative networks. The extraordinary universality of this matrix\u2010agnostic platform is validated by incredible performance increments across three distinct frontiers, driving a staggering 666% surge in combustion enthalpy for nano\u2010Al fuels, a 33% ablation reduction for ZrB\n                    <jats:sub>2<\/jats:sub>\n                    thermal shields, and concurrent \u223c270% elevations in both strength and toughness for B\n                    <jats:sub>4<\/jats:sub>\n                    C structural composites. Ultimately, this environmentally benign protocol paves a versatile avenue toward the green synthesis of high\u2010performance hybrids.\n                  <\/jats:p>","DOI":"10.1002\/advs.78222","type":"journal-article","created":{"date-parts":[[2026,10,12]],"date-time":"2026-10-12T02:56:33Z","timestamp":1791773793000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Mechanochemical Engineered Sulfur Copolymers Onto Group 13 and Related Fillers Through Lewis Acid\u2010Base Pairing"],"prefix":"10.1002","author":[{"given":"Chen","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Flexible Electronics (LOFE) &amp; Institute of Flexible Electronics (IFE) Northwestern Polytechnical University  Xi'an 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