Optically nonlinear disperse red 1 (DR1) was covalently bound into a silica gel network by the coupling of DR1 and 3-isocyanatopropyltriethoxysilane. Organic-inorganic hybrid materials present a large resonant second-order susceptibility (d33 = 55 pm/V for a fundamental wavelength of 1.06 μm) with an excellent room-temperature stability.