Inorganic-organic hybrid materials which incorporated a hemicyanine type chromophore in silica matrix were prepared by sol-gel processing technique. According to the AFM studies on the film samples of resulting hybrids, the surface roughness of both cured and poled sol-gel films was within 2 nm. The electro-optic coefficient (r 33) obtained from the different sol-gel processing conditions ranged from 1.6 to 5.0 pm/V. It was found that the sol-gel films exhibited a stable alignment of the chromophores, as observed by no decay even after 54 days.