Poly{(4-nitrophenyl)-3-[N-[2-(methacryloyloxy)ethyl]carbazolyl]] diazene} was prepared and its photoinduced birefringence, diffraction grating, and photorefractive asymmetric two-beam gain coupling were studied. The monomer was obtained by performing azo coupling in a two-phase water-dichloromethane system in the presence of a phase transfer catalyst. Photoinduced birefringence of up to 0.09 was observed and diffraction efficiencies of up to 25% were obtained, with atomic force microscopy studies revealing that the grating profile exhibited a sinusoidal shape. Asymmetric two-beam coupling is observed, indicating photorefractive properties, but the energy transfer phenomena are more complex, involving also diffraction by the photoinduced gratings. The combination of these three optical properties-photoinduced birefringence, surface gratings, and two-beam coupling-is believed to be unique and may eventually produce an all-optical device built of a single polymer film.