Internally reinforced structural composites, suitable uses for such composites, and associated methods of manufacturing are disclosed herein. In one embodiment, a method of making a reinforced structural component includes forming a precursor having a crystal structure with a plurality of lattice layers and exfoliating the precursor. As a result, a distance between adjacent pairs of the plurality of lattice layers is expanded. The method also includes wrapping the exfoliated precursor with a surface support material around at least a portion of a circumference of the individual lattice layers in the exfoliated precursor.