Carbon nanotubes (CNTs) and graphenes attract much attention as next-generation materials for semiconductor integrated circuits owing to their excellent carrier mobility and electric current durability. To be practically used, however, systematic development of fabrication processes at multiple levels is essential. In this research, an original combinatorial method is used to control molecular structures and self-organized morphologies. Facile implementation of nanocarbons with selectable higher-order structures, such as double-layer graphene for semiconducting layers, multi-walled CNT pillars for vertical wiring, and multilayer graphene ribbons for horizontal wiring, will be realized.