Developing non‐precious bifunctional electrocatalysts to drive the over water splitting that can operate well at high current densities (1,000 mA/cm2) is an urgent requirement for viable electrolysis of water. Transition metal oxides (TMO) have been intensely investigated as one of the most efficient oxygen evolution reaction (OER) catalysts. Unfortunately, their sluggish reaction kinetics towards hydrogen evolution reaction (HER) bring about poor overall performance. In this study, we perform a simple method to obtain the bifunctional TMO‐based electrocatalyst by in‐situ tailoring the components of cobalt nickel molybdenum oxide on nickel foam. By optimizing the annealing temperature and reaction atmosphere, we integrate HER‐active (CoMoNi) and OER‐active (CoMoOx) components together as bifunctional electrocatalysts for overall water splitting. Impressively, the as‐synthesized electrocatalyst shows the high electrocatalytic activity for both OER and HER, and exhibit a low cell voltage of 1.59 V at 10 mA cm−2 when applied as both the cathode and anode in alkaline solutions. Impressively, the bifunctional electrocatalysts work well at large current densities, even in the order of 1,000 mA cm−2 (only need the cell voltage of ∼2.03 V), and remain its activity more than 20 h. Such an outstanding performance should be mainly attributed to integrated high electronic conductivity, 3D self‐supported structure, and good compatibility between HER‐active and OER‐active components. This study shows a positive model for the design of more promising and practical catalysts for full water splitting.