Abstract: Embodiments of the present disclosure pertain to electrodes that include a plurality of vertically aligned carbon nanotubes and a metal associated with the vertically aligned carbon nanotubes. The vertically aligned carbon nanotubes may be in the form of a graphene-carbon nanotube hybrid material that includes a graphene film covalently linked to the vertically aligned carbon nanotubes. The metal may become reversibly associated with the carbon nanotubes in situ during electrode operation and lack any dendrites or mossy aggregates. The metal may be in the form of a non-dendritic or non-mossy coating on surfaces of the vertically aligned carbon nanotubes. The metal may also be infiltrated within bundles of the vertically aligned carbon nanotubes. Additional embodiments pertain to energy storage devices that contain the electrodes of the present disclosure. Further embodiments pertain to methods of forming said electrodes by applying a metal to a plurality of vertically aligned carbon nanotubes.