The exoskeletons of crustaceans are essential for providing protection from predators and other environmental threats. Understanding the structure and mechanical behavior of their natural armor could inspire the design of lightweight and high toughness synthetic materials. Most published work has focused on marine crustacea rather than their terrestrial counterparts, which are exposed to a multitude of unique threats. The interest in the terrestrial isopod Armadillidium vulgare (A. vulgare) has grown but the interrelationship between the microstructure, chemical composition, and mechanical properties has not been thoroughly investigated. Thus, this study aims to elucidate missing details concerning this biological mineralized composite. Exoskeleton specimens were fixated to preserve the intrinsic protein structure. We utilize scanning electron microscopy for microstructure analysis, Raman spectroscopy for elemental analysis, and nanoindentation property mapping to achieve mechanical characterization. The naturally fractured A. vulgare exoskeleton cross-section reveals four subregions with the repeating helicoidal ‘Bouligand’ arrangement most prominent in the endocuticle. The hardness and reduced modulus distributions exhibit a through-thickness exponential gradient with decreasing magnitudes from the outermost to the innermost layers of the exoskeleton. The Raman spectra show a graded spatial distribution of key constituents such as calcium carbonate across the thickness, some of which are consistent with the mechanical property gradient. Potential microstructure, elemental composition, and mechanical property relationships are discussed to explain how the hierarchical structure of this nanolaminate armor protects this species.