Supercapacitors are notable for their ability to deliver energy at higher power (compared to batteries) and store energy at higher density (compared to capacitors) as well as exhibit a long cycle life. In our efforts to further the development of supercapacitors, our focus is on using vertically aligned carbon nanotubes (VACNT) as supports for pseudocapacitive and faradaic capacitive electrode materials. The objective is to develop electrodes that can function in an inexpensive aqueous environment with relatively small potential windows, and still store energy at a higher density than carbon materials alone. We describe the different approaches explored to overcome the challenges of non-uniform deposition, poor wetting and array collapse. Materials that are electrochemically anchored to VACNT supports include Ni_xCo_yO_z, VO_x, Fe₂O₃ and Co-Mn mixed oxides. In each case, the specific capacitance obtained using the VACNT templates is more than double that obtained by direct deposition onto current collectors or by using VACNT alone as electrodes. The ease of VACNT growth and the degree of coating control that can be achieved using electrodeposition means there is much potential in exploring them as supports for capacitive electrode materials.