We demonstrated a novel method to produce core/shell composite nanowires (NWs) by self-scrolling carbon nanotubes (CNTs) onto copper NWs via forced-field-based molecular dynamic (MD) simulations. When large diameter CNTs are placed beside the copper NWs, the CNTs approach the NWs, collapse, and self-scroll onto the NWs, resulting in coaxial core/shell composite NWs. It is found that the van der Waals force plays an important role in the formation of the composite NWs. The expected outcome of this novel method is to determine various strategies on how to produce composite NWs. Coaxial core/shell composite NWs represent an important class of nanoscale building blocks with substantial potential for exploring new concepts and functional materials.