Dentin bonding based on a wet-bonding technique is the fundamental technique used daily in clinics for tooth-restoration fixation and clinical treatment of tooth-related diseases. Limited bonding durability led by insufficient adhesive infiltration in the demineralized dentin (DD) matrix is the biggest concern in contemporary adhesive dentistry. This study proposes that the highly hydrated noncollagenous protein (NCP)-formed interfacial microenvironment of the DD matrix is the root cause of this problem. Meanwhile, the endogenous phosphate groups of the NCPs are used as pseudonuclei to rapidly induce the formation of amorphous CaF