The development of multifunctional dental-restorative biomaterials with antibacterial activity and remineralization effect for damaged tooth repair is urgent since dental caries is still one of the most common tooth diseases in human beings. Herein, we report a facile strategy for the synthesis of gluey silver-calcium phosphate (GSCP) composites using the rapid microwave-assisted solvothermal method. The as-prepared GSCP composite is an organic-inorganic hybrid, and Ag+ ions display a significant influence on the formation of GSCP by interacting with adenosine triphosphate biomolecules. The as-prepared GSCP composite shows good antibacterial properties, in addition, it exhibits a great effect on sheltering dentinal canaliculi and improving the remineralization of dentine in the simulated saliva. The as-prepared GSCP composite is promising for various applications such as oral healthcare, especially, remineralization of dentine, and antibacterial applications.