Me/Al-layered double hydroxides (Me=Ni and Co) prepared by the chemical co-precipitation method have been shown to be outstanding novel materials for electrochemical capacitors. The crystalline structure and the electrochemical properties of the electrodes have been studied by considering the effect of the mole ratio of nickel/cobalt. X-ray diffraction analysis shows that the materials belong to hexagonal system with layered structure. Cyclic voltammetric measurements indicate that Me/Al-layered double hydroxides with the Ni/Co mole ratio of 4:6 exhibit excellent capacitive properties within the potential range of 0.0–0.6V versus Hg/HgO in 6mol/L KOH electrolyte. Charge/discharge behaviors have been observed with the highest specific capacitance values of 960F/g at the current density of 400mA/g. Impedance studies show that the enhanced electrical properties and high frequency response are attributed to the presence of Co oxides.