Electrochemical water splitting in alkaline solution plays a growing role in alternative energy devices due to the need for clean and sustainable energy. However, catalysts that are active for both hydrogen evolution and oxygen evolution reactions are rare. Herein, we demonstrate that cobalt phosphide (CoP), which was synthesized via the hydrothermal route and has been shown to have hydrogen evolution activity, is highly active for oxygen evolution. A current density of 10 mA cm–2 was generated at an overpotential of only 320 mV in 1 M KOH for a CoP nanorod-based electrode (CoP NR/C), which was competitive with commercial IrO2. The Tafel slope for CoP NR/C was only 71 mV dec–1, and the catalyst maintained high stability during a 12 h test. This high activity was attributed to the formation of a thin layer of ultrafine crystalline cobalt oxide on the CoP surface.