In this study, nickel and cobalt binary sulfide nanoparticles decorated on the surface of multi-walled carbon nanotubes (designated as Ni-CoS/MWCNT composite) and Ni3S2 thin films directly deposited onto Ni foam is successfully prepared by a facile glucose-assisted hydrothermal method and pulse-reversal (PR) deposition approach. On the basis of tuning the Ni/Co molar ratio of the Ni-CoS/MWCNT composites, the optimized Ni-CoS/MWCNT composite was employed as the cathode and a reduced graphene oxide was used as the anode to fabricate a hybrid supercapacitor (HSC). As-fabricated HCS is able to be operated reversibly in a full voltage region of 0–1.6 V and achieves a high specific capacity of 33 mAh g−1 at 1 A g−1. Moreover, it can still deliver a maximum energy density of 23 Wh kg−1 at a power density of 684 W kg−1. Furthermore, the HSC still retains 90% of its initial discharge capacity after 2000-cycle charge/discharge test at a fair high current density of 4 A g−1. Additionally, another HSC is then assembled by using the optimized PR-Ni3S2 electrode as cathode and carbon fiber cloth (CFC) as anode, respectively. The HSCs can be operated with a potential window between 0 and 1.8 V and deliver a high specific capacity value of 25.5 mAh g-1 at 0.5 A g-1. Moreover, the energy density and power density of the HCS can be achieved up to 28.8 Wh kg-1and 564 W kg-1, respectively. The most important thing is that the HSC displays excellent cycling stability with only 20% capacity loss after 5000 cycles. As a result, the highly efficient HSCs can be achieved based on the transition metal sulfide based materials as cathodes