Developing high-performance, robust and cost-effective oxygen evolution reaction (OER) catalysts for electrochemical water splitting is a promising way to produce energy-saving electrolytic hydrogen fuels. Herein, a series of rational wire-in-plate nanostructured CoFe LDH electrocatalysts grown on a Ni foam were developed via a one-step hydrothermal method. In this series of catalysts, Co4Fe2-LDHs/Co(OH)2-NWs exhibit excellent OER performance which is attributed to the most rational wire-in-plate nanostructure: the overpotentials of only 220 and 231 mV to drive current densities of 50 mA cm-2 and 100 mA cm-2, respectively, with a small Tafel slope of 51 mV dec-1. Our study opens up a new horizon for the design of hierarchical structures with the coexistence of multidimensional nanounits for electrocatalysts.