Poly(urethane urea) elastomers are versatile and can be tailored to exhibit a broad range of mechanical response under high strain rate deformation. In this work, we utilize coarse-grained molecular dynamics simulations to elucidate the molecular mechanisms, particularly the effects of hard segment content, intermolecular interaction, and rigidity of the interface between the hard and soft segments on local morphology and rate-dependent stress-strain behavior in the ballistic regime. Simulation results qualitatively agree with available experimental data, where analysis of hard segment orientation during tensile and compression deformation and dynamic strain rate sensitivity was also performed. Further study of the intermolecular interaction on the stress-strain behavior reveals that it has a strong effect on strain hardening, particularly for a rigid interface, once the hard segment content reaches the percolation threshold. Simulation results also show that interface intermolecular interaction could become more dominant over interface rigidity in the initial stress-strain response, particularly below percolation. Published by Elsevier Ltd.