Battery electrodes using VACNT forests to create 3D electrode nanostructures, and methods of making, are described. The VACNTs are electrically and mechanically attached to the anode or cathode substrates, providing a large area of 3D surfaces for coating with active materials and high-conductivity electron pathways to the cell current collectors. A number of different active materials suitable for anodes and cathodes in lithium-ion batteries may be used to coat the individual carbon nanotubes. The high surface area provided by the VACNT forest and the nano-dimensions of the coated active materials enable both high energy-density and high power-density to be achieved with the same battery. Complete conformal coating of the individual CNTs may be achieved by a number of different methods, and coating with multiple active materials may be used to create nanolaminate coatings having improved electrochemical characteristics over single materials.