AbstractThe dynamic mechanical properties of thermoplastic urethane elastomers have been compared for materials based on different diisocyanate structures, either 4,4′‐diphenylmethane diisocyanate (MDI) or an isomeric ratio of tolylene diisocyanate (TDI). Two comparable series of polymers were prepared with a polycaprolactone diol as the soft segment and varying concentrations of hard segments based on the respective diisocyanates and 1,4‐butanediol. Over the composition range studied, the polymer glass transition temperatures increased for the TDI‐based polyurethanes, but remained relatively constant for the series containing MDI. Differences in the degree of macroscopic order within the hard segments, due to variations in the symmetry of the diisocyanate structures, are suggested as an explanation of these dynamic mechanical pro
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