The atomic structure, charge and electronic parameters, and energies of formation of new “hybrid” nanostructures-nanopeapods Ti2@C80@C-NTs, regular linear ensembles of seven isomers of endohedral dititanofullerenes Ti2@C80 encapsulated into a carbon zigzag (19.0) nanotube—have been calculated by the self-consistent density functional tight-binding method (DFTB). The results are discussed in comparison to the “free” isomers of C80 fullerenes and Ti2@C80 endofullerenes, as well as to all-carbon nanopeapods, i.e., C80 isomers inside a carbon nanotube (C80@C-NT). It is demonstrated that the type of Ti2@C80 isomer determines the energy effect of its encapsulation into the tube (exo-or endothermic), the orientational arrangement of end-ofullerenes in the tube, the charge states of the Ti2@C80 and tube atoms, and the electronic properties of nanopeapods (semiconducting or metallic).