NiFe2O4 material is grown on carbon paper (CP) with the hydrothermal method for use as electrocatalysts in an alkaline electrolyzer. NiFe2O4 material is used as the anode and cathode catalysts (named NiFe(+)/NiFe(−) hereafter). The results are compared with those obtained using CP/NiFe as the anode and CP/Ru as the cathode (named NiFe)(+)/Ru(−) hereafter). During cell operation with NiFe(+)/Ru(−), the current density reaches 500 mA/cm2 at a cell voltage of 1.79 V, with a specific energy consumption of 4.9 kWh/m3 and an energy efficiency of 66.2%. In comparison, for NiFe(+)/NiFe(−), the current density reaches 500 mA/cm2 at a cell voltage of 2.23 V, with a specific energy consumption of 5.7 kWh/m3 and an energy efficiency of 56.6%. The Faradaic efficiency is 96–99%. With the current density fixed at 400 mA/cm2, after performing a test for 150 h, the cell voltage with NiFe(+)/Ru(−) increases by 0.167 V, whereas that with NiFe(+)/NiFe(−) decreases by only 0.010 V. Good, long-term stability is demonstrated.