Hybrid nanoparticles with unprecedented film-formability and toughness have been synthesized by simultaneous in-situ polymerization of acrylic acid and the sol-gel process of the silica precursor. The presence of two types of coupling agents (3- methacryloxypropyltrimethoxysilane (MPS) and 3- aminopropyltriethoxysilane (APTS)) provided the effective interactions between the organic and inorganic components. In addition, as evidenced by (high resolution) transmission electron microscopy (HR) TEM, the nature and concentration of coupling agent and surfactant besides the silica content played the main roles to control the morphology-dumbbell-like or core-shell- of the nanohybrids particles. Furthermore, the nanoindentation, nanoscratch and uniaxial tensile tests showed the relatively good resistance under scratch with a coefficient as low as 0.3 and a high elasticity module and hardness as large as 6.3 and 0.68 Gpa, respectively. Also, a fracture elongation up to 19% and fracture toughness up to 3.82 GJm(-3) possessed the nanohybrid comprising MPS as a coupling agent. Hence, as it was revealed from the results, the influencing parameters had a synergistic effect on the nanohybrid properties. The findings also indicated that the control of the main parameters would make it possible to control the morphology and consequently mechanical properties. (C) 2018 Elsevier Ltd. All rights reserved.