Peptide Amphiphile‐Mediated Assembly and Fusion of Anisotropic Amorphous Particles for Enamel Remineralization

Abstract Enamel remineralization, which attempts to generate a mineral layer structurally similar to native enamel and restore its mechanical properties, remains a significant challenge. Here, rationally designed peptide amphiphile (PA) molecules bind to amorphous calcium phosphate (ACP) particles via electrostatic interactions, imparting anisotropic properties that drive PA‐modified ACP to form spindle‐shaped aggregates. Furthermore, some residual PA molecules may further regulate crystallization and facilitate the formation of well‐aligned hydroxyapatite bundles. Additionally, the involvement of PA can mediate the ordered deposition and fusion of ACP on the enamel surface, and construct the crystalline‐amorphous mineralization front with a continuous structure. This mineralization front ensures epitaxially oriented growth of enamel crystals and achieves a structurally ordered mineral layer similar to that of native enamel, while the mechanical performance is effectively restored. More significantly, the thickness of the newly formed mineral layer can be augmented through cyclic remineralization, benefitting the design of products intended for practical enamel repair.