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NiFe-layered double hydroxides (NiFe-LDH) have been reported to possess exceptional oxygen evolution reaction (OER) activity. However, maintaining the stability of high activity over a long time remains a critical challenge that needs to be addressed for their practical application. Here, we report a custom-sized deep recombination of 2D graphene oxide with NiFe-LDH (NiFe-LDH/GO/NF) through a simple electrodeposition method that improves OER activity and achieves excellent stability. The excellent performance of the catalyst mainly comes from the three-phase interface and electron transport channel dredged by the three-dimensional structure constructed by the deep composite, which can not only significantly reduce its charge and electron transfer resistance, improving the material conductivity, but it also effectively increases the specific surface area, inhibits aggregation, and exposes rich active sites. In addition, GO with good conductivity not only supports NiFe-LDH well but also increases the heterogeneous interface, putting the NiFe-LDH/GO composites in close contact with Ni foam and increasing the electrocatalytic stability of the NiFe-LDH/GO/NF. The experimental results show that the overpotential of NiFe-LDH/20,000GO/NF is only 295 mV at a current density of 100 mA cm−2; the Tafel slope is 52 mV dec−1, and the charge transfer resistance (Rct) is only 0.601 Ω in 1 M KOH. This indicates that GO has excellent potential to assist in constructing geometric and electronic structures of NiFe-LDH in long-term applications. [ABSTRACT FROM AUTHOR]