Oxygen evolution reactions (OER) are often the decisive step in determining the water electrolysis rate. The first row of transition metals and their derivatives, represented by Ni and Fe, have attracted much attention due to their excellent OER performance. Here, we develop a one-step strategy for preparing oxygen-evolving electrodes, in which the NiFeOOH-modified NiFe layered double hydroxide (NiFe-LDH) nanosheet is supported by nickel foam. At 100 mA·cm−2, the overpotential of NiFeOOH-NiFe-LDH was just 227 mV, and the duration times were over 200 h in 1 mol·L−1 KOH. Furthermore, the co-existence of LDH and hydroxyl oxides helps the oxygen evolution reaction. These results suggest the potential for this synthesis strategy to provide a low-cost, highly active OER electrocatalyst for industrial water splitting.