The construction of heterogeneous interfaces and oxygen vacancy (Ov) is a very useful method to enhance the catalytic activity performance of catalysts. In this work, the high-performance a monometallic iron based bifunctional electrocatalyst FeS2/FeOOH-ZnO@NF with oxygen vacancy (Ov) and heterogeneous interface is prepared by the ZnO template induced deposition method for the first time. Due to the synergistic effect of the heterogeneous interface of FeS2/FeOOH-ZnO@NF and the oxygen vacancies of the ZnO, the FeS2/FeOOH-ZnO@NF catalysts exhibited excellent hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activity in alkaline media, with a low overpotential of 74 mV and 177 mV at 10 mA cm−2, respectively. It should be emphasized that the FeS2/FeOOH-ZnO@NF || FeS2/FeOOH-ZnO@NF electrolytic cell has an ultra-low decomposition voltage, only 1.41 V at 10 mA cm−2 and 1.49 V at 20 mA cm−2, which is much lower than that currently reported in most literatures. This work will provide a new strategy and idea for the improvement of HER and OER electrocatalytic performance of transition metal-based catalyst.