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Three model polyurethane hard segments based on dimethylol butanoic acid (DMBA) and 1,6-hexane diisocyanate (HDI), toluene diisocyanate (TDI) and 4,4-diphenylmethane diisocyanate (MDI) were prepared by the solution method.Fourier Infrared (FTIR) spectroscopy was employed to study the H-bonds in these model polyurethanes. The model polyurethane hard segment prepared from HDI and 1,4-butanodiol (BDO) was used for comparison. It was found that the H-bond but gives more H-bond patterns based on the two H-bond donors, urethane NH and carboxylic OH. The carboxylic aromatic model hard segments is stronger than that of aliphatic hard segments. The appearance of the free C = O and the fact that almost all N-H is H-bonded suggest that there possibly exist either the third H-bond acceptor or the H-bond formed by one acceptor with two donors.