The non-linear optical properties of a novel molecule, CNDA (alpha'-cyano-4'-nitrobenzal-4-N,N-dimethylaniline) were compared with that of NDA (4'-nitrobenzal-4-N,N-dimethylaniline). Guest-host type polymer films were fabricated using PMMA (polymethyl methacrylate) as matrix. Optimum corona poling temperatures of the polymer films were found to be lower than glass transition temperatures of the materials with in situ second-harmonic generation (SHG) measurement. The molecular hyperpolarizability beta of the CNDA was estimated to be about 146 x 10(-30) esu from the measured absorbance and chi((2)). The ordered CNDA also showed better stability in PMMA matrix than NDA.