As dental pulp contains the stem cells necessary for regeneration, the tooth should hold the intrinsic capacity for self-repair. A triphasic hybrid dental biocomposite (3HB) composed of biocompatible biopolymers to provide strength, antibacterial properties and protein-based cell support could provide a conducive microenvironment for the regeneration of dental structures. 3HB was incorporated into Mineral Trioxide Aggregate (ProRoot MTA) to construct a malleable injectable implant. Human tooth pulp cells (hDPCs) significantly increased proliferation in the presence of 3HB+MTA compared to 3HB or MTA alone. Cell viability decreased with MTA alone but increased with 3HB and 3HB+MTA. 3HB+MTA was implanted into the residual tooth of drilled Wistar rat M2 molars for up to 45 days. Stereological analysis from micro-CT images showed the volume of the tooth remaining. Histologically, regenerative pulpal architecture was seen invading 3HB. A continuous odontoblastic profile lined a deposit of dentin-like material suggesting reparative dentinogenesis. Overall, no infection or encapsulation was seen. Immunohistochemically, odontoblasts were seen along the margins of the wounded tooth undergoing repair. Mesenchymal cells (MSCs) were seen at the base of the drilled tooth and by 21 days had translocated into the implant itself. Cells stimulating remineralization were highly expressed in the tooth undergoing repair. CD146-positive MSCs were seen in the center of the implant, possibly stimulating remineralization. In conclusion, behavior of 3HB+ in vitro and in vivo provided a promising start as 3HB+MTA may serve as a viable regenerative scaffold for pulp regeneration; however, this should be further studied before clinical use can be considered.