Segmented poly(urethane urea) materials (PUUs) exhibit versatile mechanical properties and have drawn great interest due to their potential for protection against projectile impacts and blast loadings. To optimize the performance of PUUs for various high rate applications, specific features of their mechanical behavior have to be suitably tailored by altering the microstructure. Hence the micromechanisms governing the mechanical behavior must be identified, understood and leveraged. In this study, the effects of varying microstructure on the rate-dependent mechanical behavior were examined for select PUU materials. As expected, increasing the hard segment content increased the stiffness and the flow stress levels. Interestingly, it was observed that promoting phase mixing among the hard and soft segment domains of the PUU material greatly enhanced its rate-dependent stiffening and strain hardening behavior. These insights can help design PUUs for articles that manifest improved protective abilities under impact, while maintaining their flexibility during normal use. The potential applications for such materials are extensive, including face masks and goggles, which require excellent folding/un-folding capabilities, while also providing Superior impact resistance. Published by Elsevier Ltd.