The reversible formation of enamel-like hydroxyapatite (HA) on a dental resin microstructure remains challenging. Here, we present a poly methacryloxy propyl trimethoxy silane (MPTS)-functionalized dental resin (BTMA) that can induce reversible in situ formation of HA. The functional dental resin with silanol groups on the matrix surface was designed and prepared by photopolymerization and sol-gel processes. The role of MPTS and sol-gel process in modulating photopolymerization kinetics and the ability to induce reversible in situ HA formation were investigated using real-time Fourier-transform infrared spectroscopy, scanning electron microscopy, and energy-dispersive X-ray spectroscopy. The compression modulus of the dental resin was also conducted. The biocompatibility of BTMA was investigated by evaluating mouse preosteoblast cells (MC3T3-E1) responses to the dental material through MTT, alkaline phosphatase activity test, and osteocalcin (OCN) expression. The prepared dental material showed excellent HA generation ability in a short period of time. Once the primary mineralized HA layer on the material surface was damaged, the matrix could induce rapid in situ formation of the HA layer. Furthermore, the dental material stimulated the attachment and proliferation of MC3T3-E1 cells. Thus, our method is facile, fast, and energy conserving and can find immediate clinical application.