Cross-linked polyurethaneurea films based on polyoxytetramethylene glycol and polyoxypropylene glycol with toluene diisocyanate and 3,3 -dichloro-4,4 -diaminodiphenylmethane were synthesized in a solutionwhere the solvent evaporates during the polymerization. FT-Raman and FTIR spectra were analysed and intermolecular force constants of hydrogen bonds were calculated. On the basis of the intensity of the Raman and IR spectral lines, which reflects hydrogen bond formation, the optimum structure of hydrogen bonds and the conformations of macromolecules of polyurethaneurea were observed for the solvent ethyl acetate.