Exploring efficient, abundant, cheap and stable materials for the electrolysis of water and supercapacitor is a challenging task. Here, Ni_1−xMo_x nanosheets are obtained on carbon cloth (CC), which can be multi-functional electrodes for electrochemical applications. Impressively, we find that the electrochemical abilities can be optimized by constructing network-like nanosheets and tuning the ratio of Ni and Mo in the alloy. To acquire a current density of 10 mA cm⁻² (j₁₀), Ni_0.75Mo_0.25/CC shows the lowest overpotentials (79 mV for hydrogen evolution reaction (HER) and 330 mV for oxygen evolution reaction (OER)) in 1 M KOH. Using Ni_0.75Mo_0.25/CC as both positive and negative poles, the cell only requires a potential of 1.74 V to reach j₁₀ and shows long-term durability. We further show that Ni_0.75Mo_0.25 electrode exhibits a superior specific capacitance (422 F g⁻¹ at 1 A g⁻¹) and high capacitance retention (108.2 % after 1000 cycles) in 1 M KOH. The super-electrochemical performances of Ni_0.75Mo_0.25/CC is attributed to its high electronic conductivity, rich active sites, and large surface area. We believe that the Ni_0.75Mo_0.25/CC electrode with extraordinary electrochemical performances is a hopeful material for practical applications in both electrocatalysis and supercapacitors (SC).