Exploring efficient, abundant, cheap and stable materials for the electrolysis of water and supercapacitor is a challenging task. Here, Ni 1À x Mo 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 À 2 (j 10 ), Ni 0.75 Mo 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 0.75 Mo 0.25 /CC as both positive and negative poles, the cell only requires a potential of 1.74 V to reach j 10 and shows long-term durability. We further show that Ni 0.75 Mo 0.25 electrode exhibits a superior specific capacitance (422 F g À 1 at 1 A g À 1 ) and high capacitance retention (108.2 % after 1000 cycles) in 1 M KOH. The super-electrochemical performances of Ni 0.75 Mo 0.25 /CC is attributed to its high electronic conductivity, rich active sites, and large surface area. We believe that the Ni 0.75 Mo 0.25 /CC electrode with extraordinary electrochemical performances is a hopeful material for practical applications in both electrocatalysis and supercapacitors (SC).