This work presents the fabrication and characterization of hybrid nanostructured electrodes – polyaniline supported on a nickel nanotube array – for use in supercapacitors. Ni nanotubes were prepared using a template, and the effects of the template and preparation parameters are discussed. First, an anodized aluminum oxide (AAO) template was grown in H3PO4 under the same applied field to obtain similar pore sizes and for two different time periods to obtain different AAO thicknesses. Nickel nanotubes (Ni NTs) were prepared chemically on different AAO templates, resulting in Ni NTs of the same diameter but different lengths. A thin Ni layer was then electrodeposited on top of the Ni NTs for use as a metal contact layer in the single electrode during electrochemical tests. Vertically oriented arrays of Ni NTs on a Ni layer were obtained after etching Al and AAO. The resulting Ni NT/Ni structures were used as a substrate for electrodeposition of a polyaniline (PANI) layer at two different applied voltages. The electrodeposition parameters were chosen for homogeneous polymer deposition. The microstructural characterization of the obtained structures was carried out using a scanning electron microscope, and individual Ni nanotubes with different lengths were easily observed. The vertically oriented Ni/Ni nanotube/PANI arrays were tested for electrochemical performance (using cyclic voltammetry and impedance spectroscopy) as individual electrodes for supercapacitors. The capacitance values strongly depended on the length of the tubes and the applied current during PANI deposition and showed the highest values of 325 F/cm2 at 10 mV/s.