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Abstract Routine high strain rate impacts from the surrounding environment can cause surface erosion, abrasion, and even catastrophic failure to many structural materials. It is thus highly desirable to develop lightweight, thin, and tough impact resistant coatings. Here, inspired by the structurally robust impact surface of the dactyl club of the peacock mantis shrimp, a silicon carbide and chitosan nanocomposite coating is developed to evaluate its impact resistance as a function of particle loading. High strain rate impact tests demonstrate that coatings with 50% and 60% SiC have optimal performance with the greatest reduction in penetration depth and damage area to the substrate. Post‐impact analysis confirms that these concentrations achieve a balance between stiffness and matrix phase continuity, efficiently dissipating impact energy while maintaining coating integrity. The addition of SiC particles helps dissipate impact energy via interphase effects, particle percolation, and frictional losses due to particle jamming. The formation of these stress paths is also modeled to better understand how the addition of particles improves coating stiffness and the stress distribution as a function of particle loading. These findings highlight the potential of bioinspired materials and their promise to promote innovation and breakthroughs in the development of resilient multifunctional materials. 

We report compression tests on micropillars manufactured from bulk specimens of partially devitrified SAM2×5 (Fe_49.7Cr_17.7Mn_1.9Mo_7.4W_1.6B_15.2C_3.8Si_2.4). Yield strength values of ≈6 GPa are obtained. Such a high strength can be attributed to the higher glass transition temperature (883 K) of this material, which impedes the multiplication of shear bands under loading, and to the presence of hard crystalline domains that result from devitrification of the amorphous powders during powder consolidation. The Vickers hardness of the specimens is found to be strongly correlated to the processing temperature and, hence to the volume of crystalline phases present in the specimens. As the processing temperature is increased, there is a reduction in free volume from the structural relaxation process in the amorphous alloy, leading to the eventual nucleation of crystalline phases of BCC Fe, Cr₂B, Cr_21.30Fe_1.7C₆, or Fe₂₃B₂C₄, during the densification process. These results shed light on the relationship between nanocrystalline domains and the mechanical behavior of Fe‐based amorphous/crystalline composites.