Three kinds of ORMOSIL were obtained by one-step hydrolysis and co-condensation of tetraethyloxysilane (TEOS), together with methyltriethoxysilane (MTES), vinyltriethoxysilane (VTES), and c-glycidoxypropyltrimethoxysilane (GPTMS), respectively. IR spectra demonstrate the successful modification of silica network by methyl, vinyl, and c-glycidoxypropyl groups. The samples are mainly composed of amorphous silica phase without any detectable phase separation. The introduction of unhydrolysable organic groups retards the sol-gel process of the organoalkoxysilane and act as fillers in the silica network, leading to the condensation of the resulted ORMOSIL. Refractive index, hardness, and modulus are therefore increased.