It is of prime importance to develop dual-functional electrocatalysts with good activity for overall water splitting, which remains a great challenge. Herein, we report the synthesis of a Co-doped nickel selenide (a mixture of NiSe and NiSe)/C hybrid nanostructure supported on Ni foam using a metal-organic framework as the precursor. The resulting catalyst exhibits excellent catalytic activity toward the oxygen evolution reaction (OER), which only requires an overpotential of 275 mV to drive a current density of 30 mA cm. This overpotential is much lower than those reported for precious metal free OER catalysts. The hybrid is also capable of catalyzing the hydrogen evolution reaction (HER) efficiently. A current density of -10 mA cm can be achieved at 90 mV. In addition, such a hybrid nanostructure can achieve 10 and 30 mA cm at potentials of 1.6 and 1.71 V, respectively, along with good durability when functioning as both the cathode and the anode for overall water splitting in basic media.