Two-dimensional bi-metallic NiFe nitrides (2D NiFe-N) are successfully synthesized in the designed ternary deep eutectic solvents under the guidance of DFT calculations. Taking advantage of the unique properties of large-size, ultrathin amorphous 2D structure and modulable electronic structure, the NiFe0.05-N exhibits extraordinary OER performance with relatively low overpotential of 238 mV at 10 mA cm-2 and durable stability.