Polyurethane elastomers based on polyester diols and aromatic or aliphatic diisocyanates can be used as vibration dampers and isolation materials. Two series of cross-linked polyurethanes with various hard segment structures and different amounts were prepared and thermomechanical properties of these materials were studied. Cross-linked polyurethane copolymers composed of poly(ethylene adipate)diol as soft segment and 4,4'-methylenebis(phenylisocyanate), 1,6-hexamethylene diisocyanate, and diols glycerin, 1,4-butanediol, and 1,6-hexanediol as hard segments were synthesized by a two-step process. The networks have been prepared by end-linking a mixture of the bifunctional precursor chains with trifunctional cross-linkers at off-stoichiometric ratios. The results show that the cross-link and the polyurethane hard segment interaction play a special role in the interconnected chain density and its magnitude is revealed by the mechanical properties. Of most importance, maximum stress, tensile modulus, and elongation at break increased significantly at the 22 wt% composition of hard segment content. Interchain cross-linking improves thermal stability, which was measured by thermogravimetric analysis and differential scanning calorimetry. Cross-linked polyurethane behaves as an elastomer and is useful for shock, noise, and vibration control. (C) 2009 Wiley Periodicals, Inc. Adv Polym Techn 28: 165-172, 2009; Published online in Wiley InterScience (www.interscience.wiley.com). DOI 10.1002/adv.20155