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Abstract The core of this research is separated into three domains, the ultrahigh strain rate response of elastomeric polymers, laser‐induced shock waves , and terahertz time‐domain spectroscopy (THz‐TDS). Elastomers, e.g., polyurea, constitute an advance class of materials suitable for many applications, specifically in high impact loading scenarios, thus, a laser‐induced shock wave (LSW) experimental technique is used to investigate the mechanical response of shock‐loaded polyurea. LSW can submit samples to a strain rate exceeding 10⁶s⁻¹at low strains, enabling determination of material intrinsic failure modes. The large deformation induced during shock loading may alter the macromolecule structure, which can only be detected spectroscopically. Therefore, this research incorporated terahertz bulk spectroscopy to detect and report molecular conformational changes. Microscopy techniques were also used to elucidate changes in the microscale properties, morphology, and topography. The interpretation of the results explicated brittle failure in terms of partial and total spallation and, remarkably, ductile failure leading to plastic deformation, including plastic bulging and adiabatic shearing, not previously associated with LSW technique. Furthermore, spectral changes found in the terahertz regime substantiated the validity of terahertz spectroscopy in elucidating the underlying mechanism associated with the impact mitigating properties of dynamically loaded polyurea.