Polyurea is a versatile elastomeric thermoset that is of significant interest to the U.S. military due to its applications in blast mitigation and ballistic protection. One current challenge facing the intelligent design of polyurea polymers is its complex dynamic behavior upon blast or ballistic impact. In this work, our understanding of the structural evolution of polyurea under dynamic loading has been advanced through characterization by in-situ X-ray scattering of polyurea polymers under hydrostatic compression. It was found that under compression the hard segment domain nanocrystalline structure contracts along the interchain H-bonded urea network and recovers upon load removal. However, the extent of the recovery differed between polymers based on varying the soft segment length. We attribute this to the changing degree of phase mixing between the domains which results from the varied soft segment length. Additionally, we hypothesized that manipulating the dynamic bonding within the hard segment domains would also influence the structural evolution of polyurea under compression. In this regard we synthesized novel polyurea samples with focus on the inclusion of divalent metal cations. These cations theoretically bond to the urea linkages in the hard segments thus increasing interchain crosslinking within the polymer backbone. To evaluate the influence on the structural evolution in-situ X-ray scattering was used to characterize these samples under hydrostatic pressure. Finally, to further influence the dynamic bonding, these polymers were also modified through the substitution of additional monomers which would act as ligands for the divalent metal cations.