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Abstract Nanoparticle reinforcement is a general approach toward the strengthening of elastomer nanocomposite in large‐scale applications. Extensive studies and efforts have been contributed to demonstrating the property reinforcement of polymer nanocomposites in relation to matrix‐filler and filler‐filler interaction. Here, a facile synthetic method is creatively reported to synthesize SiO_2,15/120‐g‐polyisoprene (SiO₂‐g‐PI) particle brushes using atom transfer radical polymerization (ATRP). The dispersion and microstructures of the nanoparticles in the nanocomposites are investigated by morphological characterizations, whereas the reinforcing mechanism is studied through mechanical measurements as well as computational simulation. Remarkably, compared with the cured bulk elastomers and matrix(M)/SiO₂blends, M/particle brushes (PB) exhibit significant improvement in mechanical properties, including tensile strength, elongation at break, modules, and rolling resistance. This elastomer nanocomposites afford a novel prospect for the practical application of next‐generation automobile tires with enhanced performance.