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By in situ grafting methacroyloxy functionalized silanes on commercial nanoglobular silica polymerization‐active silico‐organic nanoparticles were prepared. In radiation (UV, EB) induced polymerization reactions these modified nanoparticles form covalent crosslinks to acrylate substrates, thus efficiently modifying their viscoelastic properties. The transparent nanopowder composites can be used as scratch resistant coatings. The composite films show excellent adhesion on PC and PVC and good abrasion resistance after the Taber abraser test with haze values of about 6% after 500 cycles.