Mechanical response of polyurea, a nanophase segregated elastomeric co-polymer, is investigated using all-atom, equilibrium, molecular-dynamics methods and tools. Specifically, the effects of high pressure (1-30 GPa) and high strain rate (10(5)-10(6) s(-1)) on the shearing resistance of polyurea are examined. Such loading conditions are encountered by polyurea coatings subjected to impact by high-velocity projectiles, shell shrapnel, and improvised explosive device fragments. Computed results are compared with their experimental counterparts obtained using the so-called pressure-shear plate impact experiments. Computed results have also been rationalized in terms of the nanosegregated polyurea microstructure consisting of rod-shaped, discrete, the so-called hard domains embedded in a highly compliant, the so-called soft matrix. By analyzing molecular-level microstructure and its evolution during high-rate deformation and under high imposed pressures, an attempt is made to identify and quantify main phenomena in viscous/inelastic deformation and microstructure-reorganization processes that are most likely responsible for the observed mechanical response of polyurea.