Composite materials with Ti or Ti alloy reinforcement in a Zn matrix are new, promising materials with potential applications in implantology. Infiltrating zinc into the porous titanium reinforcement of a designed implant could improve its osseointegration. In this field, it is important to avoid the formation of brittle intermetallics; therefore, understanding their growth is fundamental. This work focuses on characterizing the Ti-Zn intermetallic phases at the interface of the TiAlV/Zn and Ti/Zn composites. Samples were prepared by immersing the Ti-6Al-4V or Ti bulk material in zinc melt at various temperatures. After various dwell times, the samples (pieces of Ti-6Al-4V or Ti in the molten zinc) were removed from the furnace and cooled in air. The sequence of evolution of intermetallic phases was observed to be dependent on dwell time at selected temperatures. The influences of surface treatment methods on the boundary structure were also tested.