Supercapacitors are known as promising excellent electrochemical energy storage devices because of their attractive features, including quick charge and discharge, high power density, low cost and high security. In this work, a series of litchi-like Ni-Co selenide particles were synthesized via a simple solvothermal method, and the Ni-Co compositions were carefully optimized to tune the charge storage performance, charge storage kinetics, and conductivity for battery-like supercapacitors. Interestingly, the optimal sample Ni 0.95 Co 2.05 Se 4 exhibits a high capacity of 1038.75 F g −1 at 1 A g −1 and superior rate performance (retains 97.8% of the original capacity at 4 A g −1 ). Moreover, an asymmetric supercapacitor device was assembled based on the Ni 0.95 Co 2.05 Se 4 cathode and activated carbon anode. The device of Ni 0.95 Co 2.05 Se 4 //active carbon (AC) reveals a peak energy density of 37.22 W h kg −1 , and the corresponding peak power density reaches 800.90 W kg −1 . This work provides a facile and effective way to synthesize transition metal selenides as high-performance supercapacitor electrode materials. The litchi-like Ni-Co selenide constructed Ni 0.95 Co 2.05 Se 4 //AC hybrid supercapacitor achieves an energy density of 37.22 W h kg −1 and a power density of 800.90 W kg −1 . The ASC device can retain 95.21% of the original capacity after 4000 cycles.