Nature is filled with materials that are both strong and light, such as bones, teeth, bamboo, seashells, arthropod exoskeletons, and nut shells. The insights gained from analyzing the changing chemical compositions and structural characteristics, as well as the mechanical properties of these materials, have been applied in developing innovative, durable, and lightweight materials like those used for impact absorption. This research concentrates on the involucres of Job’s tears (Coix lacryma-jobi var. lacryma-jobi), which are rich in silica, hard, and serve to encase the seeds. The chemical composition and structural characteristics of involucres were observed using scanning electron microscopy and energy-dispersive x-ray spectroscopy and optical microscopy with safranin staining. The hardness of the outer and inner surfaces of the involucre was measured using the micro-Vickers hardness test, and the Young’s modulus of the involucre’s cross-section was measured using nanoindentation. Additionally, the breaking behavior of involucres was measured through compression test and three-point bending tests. The results revealed a smooth transition in chemical composition, as well as in the orientation and dimensions of the tissues from the outer to the inner layers of involucres. Furthermore, it was estimated that the spatial gradient of the Young’s modulus is due to the gradient of silica deposition. By distributing the hard, brittle silica in the outer layer and elastoplastic organic components in the middle and inner layers, the involucres effectively respond to compressive and tensile stresses that occur when loads are applied to the outside of the involucre. Furthermore, the involucres are reinforced in both meridional and equatorial directions by robust fibrovascular bundles, fibrous bundles, and the inner layer’s sclerenchyma fibers. From these factors, it was found that involucres exhibit high toughness against loads from outside, making it less prone to cracking.