Graphene was grown directly on porous nickel films, followed by the growth of controlled lengths of vertical carbon nanotube (CNT) forests that seamlessly emanate from the graphene surface. The metal-graphene-CNT structure is used to directly fabricate field-emitter devices and double-layer capacitors. The three-dimensional nanostructured hybrid materials, with better interfacial contacts and volume utilization, can stimulate the development of several energy-efficient technologies.