MnO2-pillared layered manganese oxide has been first fabricated by a delamination/reassembling process followed by oxidation reaction and then by heat treatment. The structural evolution of MnO2-pillared layered manganese oxide has been characterized by XRD, SEM, DSC-GTA, IR and N2 adsorption-desorption. MnO2-pillared layered manganese oxide shows a relative high thermal stability and mesoporous characteristic. The layered structure with a basal spacing of 0.66nm could be maintained up to 400°C. The electrochemical properties of the synthesized MnO2-pillared layered manganese oxide have been studied using cyclic voltammetry in a mild aqueous electrolyte. Sample MnO2–BirMO (300°C) shows good capacitive behavior and cycling stability, and the specific capacitance value is 206Fg−1.