Manganese oxide powders were prepared by spray pyrolysis from manganese acetate solution with various pyrolysis temperatures and directly collected via high-voltage electrostatic deposition technique (ESD). The as-prepared powders were coated onto graphite substrates by electrophoretic deposition technique (EPD). The as-prepared powders and/or coatings were examined by X-ray diffractometry (XRD), Fourier transform infrared spectroscopy (FTIR), cyclic voltammetry (CV), and etc. XRD data determined the phase of the as-prepared powders as nanocrystalline Mn3O4 phase, manganese hydroxide and residual acetate. In addition, the electrochemical characteristics of the resulting powder mixtures were examined by cyclic voltammetry and charge/discharge cycling in electrolyte for redox supercapacitor applications.