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Electrochemical pseudocapacitors, along with batteries, are the essential components of today's highly efficient energy storage systems. Cobalt oxide is widely developing for hybrid supercapacitor pseudocapacitance electrode applications due to its wide range of redox reactions, high theoretical capacitance, low cost, and presence of electrical conductivity. In this work, a recovery annealing approach is proposed to modify the electrochemical properties of Co 3 O 4 pseudocapacitive electrodes. Cyclic voltammetry measurements indicate a predominance of surface-controlled redox reactions as a result of recovery annealing. X-ray diffraction, Raman spectra, and XPES results showed that due to the small size of cobalt oxide particles, low-temperature recovery causes the transformation of the Co 3 O 4 nanocrystalline phase into the CoO phase. For the same reason, a rapid reverse transformation of CoO into Co 3 O 4 occurs during in situ oxidation. This recrystallization enhances the electrochemical activity of the surface of nanoparticles, where a high concentration of oxygen vacancies is observed in the resulting Co 3 O 4 phase. Thus, a simple method of modifying nanocrystalline Co 3 O 4 electrodes provides much-improved pseudocapacitance characteristics.