A new series of Y-type polyurethanes containing different concentrations of nonlinear optical (NLO) chromophore with aniline donor and tricyanofurane (TCF) acceptor have been successfully prepared, and characterized by FTIR, UV-Vis, and 1H-NMR spectra. New polyurethanes were synthesized with different chromophore contents by introducing diol N, N-dihydroxyethylaniline or 4-[N, N-(dihydroxyethyl)amino]benzaldehyde. These NLO polyurethanes exhibit good film forming property and high thermal stability up to 281 degrees C. The highest electro-optic coefficient (r33) of polymers is up to 39 pm V1 measured by simple reflection technique at 1310 nm, and the temporal stability of the poling-induced order at elevated temperature of 80 degrees C was much improved through the introducing of hydrogen bonding interaction in this system. (c) 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013