The shape-controlled synthesis of NiCo2 O4 microstructures through a facile hydrothermal method and subsequent calcinations was explored. By employing CoSO4 , NiSO4 , and urea as the starting reactants, flower-like NiCo2 O4 microstructures were obtained at 100 °C after 5 h without the assistance of any additive and subsequent calcination at 300 °C for 2 h; dumbbell-like NiCo2 O4 microstructures were prepared at 150 °C after 5 h in the presence of trisodium citrate and subsequent calcination at 300 °C for 2 h. The as-prepared NiCo2 O4 microstructures were characterized by X-ray powder diffraction, field-emission scanning electron microscopy, energy-dispersive X-ray spectroscopy, and (high-resolution) transmission electron microscopy. Both the flower-like and dumbbell-like NiCo2 O4 microstructures could be used as electrode materials for supercapacitors, and they exhibited excellent electrochemical performance, including high specific capacitance, good rate capability, and excellent long-term cycle stability. Simultaneously, the shape-dependent electrochemical properties of the product were investigated.