Four novel segmented polyurethanes (PUs) based on4,4-{oxy-1,4-diphenyl bis(nitromethylidine)}diphenol (ODBNMD) diol with different diisocyanates such as 4,4-diphenylmethane diisocyanate, toluene 2,4-diisocyanate, isophorone diisocyanate, and hexamethylene diisocyanate have been prepared by solution method. The structures of ODBNMD and PUs have been confirmed by Fourier transform infrared (FTIR), nuclear magnetic resonance (H-1-NMR and C-13-NMR), UV-visible, and fluorescence spectroscopies. The segmented PUs were further characterized by thermogravimetry (TGA), differential scanning calorimetry (DSC), and wide-angle X-ray diffraction. FTIR confirmed hydrogen bonding interactions, whereas TGA and DSC suggested that introduction of aromatic/phenyl ring in the main chain considerably increased the thermal stability. POLYM. ENG. SCI., 54:24-32, 2014. (c) 2013 Society of Plastics Engineers