This article reports the structure and morphology of the in vivo interface between implants composed of either a tricalcium phosphate (αTCP) or αTCP doped with 3.0 wt% dicalcium silicate (αTCP(ss)) ceramic, and natural bone of rabbit tibias. Both interfaces developed a new bone layer in direct contact with the implants after 4 and 8 weeks of implantation. The specimens were examined using analytical scanning and transmission electron microscopy, up to the lattice plane resolution level. Degradation processes of the implants developed at the interfaces encouraged osseous tissue ingrowth into the periphery of the material, changing the microstructure of the implants. The ionic exchange initiated at the implant interface with the environment was essential in the integration process of the implant, through a dissolution–precipitation–transformation mechanism. The interfaces developed normal biological and chemical activities and remained reactive over the 8-week period. Organized collagen fibrils were found at the αTCP(ss)/bone interface after 4 weeks, whereas a collagen-free layer was present around the Si-free αTCP implants. These findings suggest that the incorporation of silicate ions into αTCP ceramic promotes processes of the bone remodeling at the bone/αTCP(ss) interface, hence the solubility rate of the aTCP(ss) material decreased.