Abstract Polyurethanes were prepared from toluene diisocyanate (TDI), 1-4-butane diol (BDO) and polycaprolactone-based triols with varying molecular weights. Among each molecular weight triol-based urethane, hard segment content was varied from 20% to 70%. Differential scanning calorimetry, tensile testing, and Iosipescu shear testing were done on all the various urethanes prepared. Thermal characterization data revealed the dependence of phase separation on hard segment content as well as on the triol molecular weight. Tensile data and Iosipescu shear data further confirmed the observations made from the DSC data. The data further indicated that phase separation can greatly improve the modulus of cross-linked segmented urethanes. Adhesion of these urethanes to glass surface was evaluated using soda-lime float glass plate. Urethane samples were cast on the air side of the glass plates and adhesion was measured in shear mode. Adhesion data indicated that in addition to hard segment content, modulus, cross-...