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Exploitation of oxygen evolution reaction (OER) and urea oxidation reaction (UOR) catalysts with high activity and stability at large current density is a major challenge for energy-saving H2 production in water electrolysis. Herein, we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe2O4 (FeNi/NiFe2O4@NC) for efficiently increasing the performance of water and urea oxidation. Due to the tensile strain effect on FeNi/NiFe2O4@NC, it provides a favorable modulation on the electronic properties of the active center, thus enabling amazing OER (η100 = 196 mV) and UOR (E10 = 1.32 V) intrinsic activity. Besides, the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density, showing high industrial practicability. This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.