Fundamental understanding of high strain rate deformation behavior of materials is critical in designing new alloys for wide-ranging applications including military, automobile, spacecraft, and industrial applications. High entropy alloys, consisting of multiple elements in (near) equimolar proportions, represent a new paradigm in structural alloy design providing ample opportunity for achieving excellent performance in high strain rate applications by proper selection of constituent elements and/or thermomechanical processing. This dissertation is focused on fundamental understanding of high strain-rate deformation behavior of several high entropy alloy systems with widely varying microstructures. Ballistic impact testing of face centered cubic Al0.1CoCrFeNi high entropy alloy showed failure by ductile hole growth. The deformed microstructure showed extensive micro-banding and micro-twinning at low velocities while adiabatic shear bands and dynamic recrystallization were seen at higher velocities. The Al0.7CoCrFeNi and AlCoCrFeNi2.1 eutectic high entropy alloys, with BCC and FCC phases in lamellar morphology, showed failure by discing. A network of cracks coupled with small and inhomogeneous plastic deformation led to the brittle mode of failure in these eutectic alloys. Phase-specific mechanical behavior using small-scale techniques revealed higher strength and strain rate sensitivity for the B2 phase compared to the L12 phase. The interphase boundary demonstrated good stability without any cracks at high compressive strain rates. The Al0.3CoCrFeNi high entropy alloy with bimodal microstructure demonstrated an excellent combination of strength and ductility. Ballistic impact testing of Al0.3CoCrFeNi alloy showed failure by ductile hole growth and demonstrated superior performance compared to all the other high entropy alloy systems studied. The failure mechanism was dominated by micro-banding, micro-twining, and adiabatic shear localization. Comparison of all the high entropy alloy systems with currently used state-of-the-art rolled homogenous armor (RHA) steel showed a strong dependence of failure modes on microstructural features.