Multi-pass friction stir processing (FSP) was used to obtain a titanium alloy/copper hybrid composite layer by intermixing copper powder with a Ti6Al4V alloy. A macrostructurally inhomogeneous stir zone was obtained with both its top and middle parts composed of fine dynamically recrystallized α- and b-Ti grains, as well as coarse intermetallic compounds (IMCs) of Ti2Cu and TiCu2, respectively. Some b grains experienced β → α a decomposition with the formation of acicular α-Ti microstructures either inside the former b-Ti grains or at their grain boundaries. Both types of β → α a decomposition were especially clearly manifested in the vicinity of the Ti2Cu grains, i.e., in the copper-lean regions. The middle part of the stir zone additionally contained large dislocation-free b-Ti grains that resulted from static recrystallization. Spinodal decomposition, as well as solid-state amorphization of copper-rich b-Ti grains, were discovered. The FSPed stir zone possessed hardness that was enhanced by 25% as compared to that of the base metal, as well as higher strength, ductility, and wear resistance than those obtained using four-pass FSPed Ti6Al4V.