Polyphasic calcium phosphates (Poly-CaP), a complex of hydroxyapatite (HAp) and soluble calcium phosphates including α-tricalcium phosphate and tetracalcium phosphate, demonstrate promoting effects on hard tissue formation by osteoblasts. We hypothesized that a Poly-CaP block with a soluble calcium phosphates phase on one side and an insoluble HAp phase on the other side is useful for vital pulp therapy as it may promote dentin regeneration and provide the surface effective to achieve sealing. The purpose of this study was to investigate the efficacy of Poly-CaP as a direct pulp capping material by examining the Ca-release profile, the in vivo ability to induce reparative dentinogenesis, and the bonding of HAp surface with adhesive systems