Updated project metadata. Radula is a unique foraging organ to Mollusca, which is important for their evolution and taxonomic classification. Many radulae are mineralized with metals. Although the remarkable mechanical properties of mineralized radula are well-studied, the formation of mineralization from nonmineralized radula is poorly understood. Taking advantage of the recently sequenced octopus and chiton genome, we were able to identify more species-specific radula proteins by proteomics. Comparing these proteomes enable us to gain insight into the molecular components of nonmineralized and mineralized radula, highlighting that iron mineralization in chiton radula is possibly due to the evolution of ferritins and peroxiredoxins. Through in vitro binding assay, ferritin is shown to be important to iron accumulation into the nonmineralized radula. Moreover, radula proteomes are well adapted to their functionality. Octopus radula has many scaffold modification proteins to suit flexibility while chiton radula has abundant sugar metabolism proteins (e.g. glycosyl hydrolases) to adapt to algae feeding. This study provides a foundation for the understanding of Mollusca radula formation and evolution and may inspire the synthesis of iron nanomaterials.