Constructing the Enamel-Like Dentin Adhesion Interface to Achieve Durable Resin-Dentin Adhesion. ACS nano Enamel adhesion is acknowledged as durable; however, achieving long-lasting dentin adhesion remains a formidable challenge due to degradation of exposed collagen matrix after acid-etching of dentin. The idea of developing an enamel-like adhesion interface holds great promise in achieving enduring dentin adhesion. In this study, we constructed an enamel-like adhesion interface using a rapid remineralization strategy comprising an acidic primer and a rapid remineralization medium. Specifically, the acidic primer of 10-methacryloyloxydecyl dihydrogen phosphate (MDP) and epigallocatechin-3-gallate (EGCG) nanocomplex (MDP@EGCG primer) was utilized to partially demineralize dentin within 30 s, and the MDP@EGCG nanocomplex showed a strong interaction with exposed collagen, enhancing collagen remineralization properties. Then, the rapid remineralization medium containing polyaspartate (Pasp) stabilized amorphous calcium and phosphorus nanoclusters (rapid Pasp-CaP) was applied to modified dentin collagen for 1 min, which caused rapid collagen remineralization within a clinically acceptable time frame. This strategy successfully generated an inorganic rough and porous adhesive interface resembling etched enamel, fundamentally addressed issues of collagen exposure, and achieved durable dentin adhesion and while also ensuring user-friendliness. It exhibited potential in prolonging the lifespan of adhesive restorations in clinical settings. In addition, it holds significant promise in the fields of caries and dentin sensitivity treatment and collagen-based tissue engineering scaffolds. 10.1021/acsnano.4c11224