Since the complicated multiple electron transfer process and slow kinetics in the OER process seriously hinder the electrochemical decomposition of water, it is urgent to design and develop electrocatalysts with excellent performance and superior stability to reduce overpotential and accelerate the reaction dynamics of the OER. Herein, a unique ultra-thin nanosheet bimetal electrocatalyst NiFe-MOF/IF was synthesized by a one-step hydrothermal method, and characterized by SEM, XRD, TEM, and XPS. NiFe-MOF/IF shows superior OER electrocatalytic activity in 1 M KOH electrolyte solution, and an ultralow overpotential of only 230 and 262 mV was required to achieve a current density of 10 and 100 mA cm, respectively, with a relatively small Tafel slope of 30.46 mV dec for the OER. No obvious degradation of the current density at 10 mA cm was observed over about 16 h, which indicates the excellent stability of the catalyst. Favourable activity and benign durability of NiFe-MOF/IF can be attributed to the three-dimensional high porosity conductive substrates, in situ growth of MOF nanosheets, bimetallic synergy, and unique layering. This research provides a promising strategy for the application of MOF materials in the field of electrocatalysis.