SynopsisThe morphology of a chemically crosslinked urethane elastomer is correlated with its time-dependent mechanical properties. Evaluation of this amorphous elastomer by electron microscopy and small-angle x-ray scattering reveals that incompatible chain segments cluster into separate microphases having a periodicity in electron density of about 90 A. This observed domain structure is similar to that seen previously in uncrosslinked, thermoplastic urethane elastomers. As in earlier studies on such linear systems, thermal pretreatment of the crosslinked elastomer causes a timedependent change in its room temperature modulus. However, the magnitude of this modulus change (about 2W) is generally less than observed previously with the linear systems. Another contrast with previous findings is that this time-dependent phenomenon is apparently not caused by thermally activated changes in microphase segregation. Rather, the observed time dependence in modulus is believed to be caused by molecular relaxation resulting in densification of amorphous packing within the hard-segment domains. The validity of this proposed mechanism is supported by differential scanning calorimetry experiments showing evidence of enthalpy relaxation during roomtemperature aging of the elastomer. This relaxation is qualitatively similar to that observed previously during sub-T, annealing of single-phase glassy polymers.