Dual-functional NiCo2S4 polyhedral architectures with outstanding electrochemical performance for supercapacitors and lithium-ion batteries (LIBs) have been rationally designed and successfully synthesized by a hydrothermal method. The as-synthesized NiCo2S4 electrode for supercapacitor exhibits an outstanding specific capacitance of 1298Fg-1 at 1Ag-1 and an excellent rate capability of ~80.4% at 20Ag-1. Besides, capacitance retention of 90.44% is realized after 8000 cycles. In addition, the NiCo2S4 as anode in LIBs delivers high initial charge/discharge capacities of 807.6 and 972.8mAhg-1 at 0.5C as well as good rate capability. In view of these points, this work provides a feasible pathway for assembling electrodes and devices with excellent electrochemical properties in the next generation energy storage applications.