This work is based on developing an amorphous silicon-coated, vertically aligned carbon nanotube (CNT) forest for energy storage applications. The architecture of the electrode has three valuable features: (1) enhanced charge transfer via aligned CNTs to the substrate, (2) excellent charge storage capability via amorphous silicon, and (3) the preservation of high surface area and porosity with enhanced energy storage capacity. As such, this work could offer a new type of nanomaterial for energy storage applications. A supercapacitor electrode is used in this work for the energy storage demonstration.