Most biological materials are hierarchically structured composites that often possess exceptional mechanical properties. We show that nanoindentation can be a powerful tool for understanding the structure‑mechanical property relationship of biological materials and illustrate this for fish teeth and scales, not heretofore investigated at the nanoscale. Piranha and shark teeth consist of enameloid and dentin. Nanoindentation measurements show that the reduced modulus and hardness of enameloid are 4‑5 times higher than those of dentin. Arapaima scales are multilayered composites that consist of mineralized collagen fibers. The external layer is more highly mineralized, resulting in a higher modulus and hardness compared with the internal layer. Alligator gar scales are composed of a highly mineralized external ganoin layer and an internal bony layer. Similar design strategies, gradient structures, and a hard external layer backed by a more compliant inner layer are exhibited by fish teeth and scales and seem to fulfill their functional purposes.