Designing and synthesizing proper electrocatalysts with bifunctions for hydrogen and oxygen generation catalytic activity remains a great challenge. In this manuscript, we successfully develop and fabricate an earth abundant Ni-Mo-S based electrocatalyst that is bifunctionally active for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by water splitting in alkaline electrolyte (1M NaOH). Such an electrocatalyst demonstrates the capability for water splitting in alkaline electrolyte with an applied potential of 1.539 V at the current density of 10 mA/cm2 when used as both anode and cathode. Though detailed studies in the reaction mechanism are still further required, the results suggest that the geometrical high surface area and the modified electronic structures and surface chemistry are very important in designing bifunctional electrocatalysts.