Thin films of the nonlinear optical material 4′‐nitrobenzylidene‐3‐acetamino‐4‐methoxy‐aniline have been prepared using the organic molecular beam deposition technique. High quality homoepitaxial layers have been grown at substrate temperatures of 80 °C and moderate growth rates of 0.1–0.5 A˚/s. The samples have been characterized by optical polarization and interference microscopy as well as atomic force microscopy. Growth experiments on inorganic substrates, including silicon and glass, have been performed in a substrate temperature range of −190 to 100 °C and led to amorphous films at low temperatures and polycrystalline films at temperatures above 50 °C. ©1995 American Institute of Physics.