A solvent free, highly concentrated silica-acryl monomer hybrid sol was synthesized using aqueous colloidal silica as a precursor. The effects of the silica particle size, type of surface treatment agent employed, and silica content on the formation of the hybrid sol were systematically studied. The optical and physical properties of the coating solution prepared using the hybrid sol were also characterized. The viscosity of the hybrid sol tended to decrease as the particle size of the silica and the molecular weight of the surface treatment agent increased. The PET substrate coated with MPTMS-Mix (mixture, 70 wt%) solution showed the highest surface hardness (6 H) and low surface roughness (Ra= 0.044 μm), which could be attributed to an increase in packing density caused by the infiltration of small particles into the pores formed between larger particles.