Teeth are important for our life, and enamel, as the outermost layer of the tooth, plays a key role in maintaining the function and health of the tooth. Regeneration of acid eroded enamel is a big challenge due to the lack of living cells in the enamel. Here, we propose a novel way to chemically synthesize the enamel structure by mimicking the interaction of amorphous calcium phosphate (ACP) and acidic proteins during the formation of natural enamel. The process includes the formation of ACP in situ by acid etching and then the formation of a Ca-rich polypeptide-ACP complex on acid etched enamel apatite crystals, the oriented nucleation and growth of apatite nano-crystals along the acid etched enamel apatite crystals, and infiltration of a regenerated enamel apatite structure with dental resin. The synthesized enamel reveals not only excellent mechanical properties, which are highly close to those of original natural enamel, but also reveals high chemical stability against acid erosion. This innovative method may create potential applications of the functional artificial enamel for repairing damaged tooth enamel.