We report a microwave-assisted synthesis of a self-assembled three-dimensional graphene-carbon nanotube-nickel (3D G-CNT-Ni) nanostructure, which can be used as a high capacity anode material in lithium-ion batteries (LIBs). The unique 3D G-CNT-Ni nanostructure shows that CNTs are grown on graphene sheets through tip growth mechanism by Ni nano-particles. Bunches of CNTs and graphene sheets produce 3D network nanostructures with ultrahigh surface area, a large number of activation sites, and efficient ion pathways, all of which are crucial for high capacity anode materials in LIBs. The synthesized 3D nanostructure maintains a reversible specific capacity of 648.2 mA h/g after 50 cycles at a current density of 100 mA/g, as high capacity electrode structures in LIBs. (c) 2013 Elsevier Ltd. All rights reserved.