We prepared the photorefractive sol-gel glass based on organic-inorganic hybrid materials containing a charge transporting molecule, second-order nonlinear optical chromophore, photosensitizer, and plasticizer. Carbazole and 2-{4-[(2-hydroxyethyl) methylamino]benzylidene}malononitrile were reacted with 3-isocyanatopropyl triethoxysilane and the functionalized silanes were employed to fabricate the efficient photorefractive media including 2,4,7-trinitrofluorenone (TNF) to form a charge transfer complex. The simplest way to vary the composition in the matrix was to mix the desired amount of the functionalized alkoxysilane. The prepared sol-gel glass samples contained a large amount of nonlinear optical (NLO) chromophore compared to that of the charge transporting molecules. They showed a large net gain coefficient and high diffraction efficiency at certain conditions.