A nonlinear optical waveguide with organic crystals based on 4-nitrobenzyliden-3acetamino-4-methoxyaniline (MNBA) and its derivative was fabricated by organic molecular-beam epitaxy and operated as an electro-optic (EO) device. It has been proved that an EO coefficient r11 of MNBA significantly depends on the thickness of the 4-nitrobenzyliden3-ethylcarbonylamino-4-methoxyaniline (MNBA–Et) homoepitaxial layer. Insertion of a thicker MNBA–Et homoepitaxial layer enlarges r11 of MNBA heteroepitaxial layer from 30 to more than 150 pm/V.

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