Cobalt sulfide (Co9S8) particles are compounded as the electrode materials of supercapacitors by a mechanical alloying method. They show excellent properties including good cycling stability and high specific capacitance. A supercapacitor is assembled using Co9S8 as the anode and activated carbon (AC) as the cathode. It gains a maximum specific capacitance of 55 F·g−1 at a current density of 0.5 A·g−1, and also an energy density of 15 Wh·kg−1. Those results show that the novel and facile synthetic route may be able to offer a new way to synthesize alloy compounds with excellent supercapacitive properties.