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Abstract: Chemical anchoring of silica nanoparticles onto polyaniline (PANI) chains was conducted through electro-co-polymerization of aniline and N-substituted aniline grafted on surfaces of silica nanoparticles. The grafting of N-substituted aniline on surfaces of silica nanoparticles were realized through hydrolysis of triethoxysilylmethyl N-substituted aniline (ND42) and the following condensation reaction with silanol groups on surfaces of SiO2. Organic–inorganic interactions between PANI and SiO2 involved in electro-co-polymerization process pushed the polymer chains apart and so facilitated the 1D growth of the polymer. Hence, the obtained hybrid film PANI/ND42–SiO2 displayed nano-fibrous morphologies (ca. 50nm in diameter). Consequently, PANI/ND42–SiO2 exhibited an average specific capacitance of 380Fg−1, ca. 40% higher than that of PANI/SiO2 (276Fg−1). The hybrid film also showed improved cyclic stability. [Copyright &y& Elsevier]