Chitons and limpets harden their teeth with biominerals in order to scrape algae from hard rock surfaces. To elucidate relationships between tooth structure and function, light and electron microscopy were used to examine naturally worn teeth in three species of mollusc with iron-mineralized teeth and to analyze the grazing marks left by members of these species feeding on wax. For the two chiton species, teeth wore down progressively from the medial to the lateral edge of the cusp, while for the limpet, wear was more evenly distributed across the edges of each cusp. In chitons, this pattern of wear matched the medially biased morphology of the cusps in their protracted position and relates to what is known about the mineral composition and substructure of the teeth. The patterns of progressive tooth wear for each of these species, together with the distinct grazing marks left by each species on the wax substrate, indicate that the teeth are designed to remain functionally effective for as long as possible, and have proved to be a valuable means of rationalizing the internal architecture of the teeth at a range of spatial scales. This information is critical for ongoing studies aimed at understanding the interactions between the organic matrix and mineral components of these teeth.