A novel MnO2-pillared Ni2+-Fe3+ layered double hydroxides nanocomposite has been successfully fabricated using an intercalation/reduction reaction followed by heating treatment. The structural evolution of the samples obtained at different stages has been characterized by XRD, TEM, XPS, IR and N-2 adsorption-desorption. The layered structure of MnO2-pillared Ni2+-Fe3+ layered double hydroxides nanocomposite can be maintained at 300 degrees C, and the obtained material has a large surface area of 202 m(2) g(-1). Electrochemical studies indicate that the material obtained by heating at 200 degrees C exhibits an ideal capacitive behavior and good cycling property in 1 mol L-1 Na2SO4 aqueous solution, and the specific capacitance value was 190 F g(-1) at a scan rate of 5 mV s(-1). (c) 2010 Elsevier Inc. All rights reserved.