A simple and novel strategy has been developed for the morphology-controlled synthesis of hierarchical CoS2 microspheres. The hierarchical mesoporous CoS2 architecture constructed by ultrathin nanosheets, when applied as electrode materials for supercapacitors, achieves a highest specific capacitance of 718.7Fg−1 at 1Ag−1 under a high mass loading, excellent rate capability (66.3% capacitance retention from 1Ag−1 to 20Ag−1), and good cycling stability (only a loss of 7.0% in the specific capacitance after 1000 cycles). Therefore, this work provides a promising approach for the rational design and synthesis of morphology-tunable micro/nanomaterials with superior properties for supercapacitors and other electrochemical applications.