It has been challenging for metals to synthesize optimal nano- structures with a desirable performance. Herein, we propose a new idea for the development of nano-network structures in Al/C60 composites by the self-assembly of Al-C phases. Carbon atoms, dissembled from the individually dispersed C 60-fulIerenes, are intercalated into the interstitials of aluminum, producing Al-C phases with artificially moderated lattice structures. The isolated Al-C phases grow with a strong anisotropy derived from lattice mismatch, meet neighbor Al-C phases, and then self-assemble into network structures. The novel nano-structures, extremely stable at high temperatures, offer significant potential for the development of thermally-stable high-strength structural aluminum. The controlled lattice provides a new paradigm for atomic level design of crystalline materials.