This chapter is devoted to the study of the electronic structure and electrical properties of two-dimensional (2D) films based on carbon nanotube/graphene composite with horizontal packing of tubes between graphene sheets. The influence of topology—the chirality of nanotubes and the distance between them—on the electron energy and electrical characteristics of the composites is studied. To reveal new physical regularities of the hybrid carbon nanostructures under consideration, numerical experiments have been performed using quantum mechanical and molecular dynamics methods.