Nanostructured ε-manganese dioxide films are deposited directly on three-dimensional nickel foam (NF) from 0.25 M Mn(CH3COO)2 by means of the potentiostatic method (PSM) and potentiodynamic method (PDM). The prepared MnO2 films are characterized by X-ray diffraction and scanning electron microscopy. The electrochemical properties of MnO2 films are investigated by cyclic voltammetry (CV), charge-discharge tests, and alternating current (AC) impedance spectroscopy. The results show that the PSM-MnO2 films exhibit higher specific capacitance and better high-rate discharge ability, which are more promising for applications in supercapacitor than PDM-MnO2 films. The specific capacitance of PSM-MnO2 films is about 664 F g-1 at 5.5 A g-1, which is higher than many reported values.