AbstractThe oxygen evolution reaction (OER) is crucial for hydrogen production. However, OER with four‐electron transfer requires electrocatalysts to speed up its sluggish kinetics in alkaline solutions. Herein, amorphous CoV phosphate (denoted as CoV−Pi) nanosheets synthesized by a straightforward one‐step hydrothermal approach is reported, which provide a low overpotential of 320 mV at 10 mA cm⁻², a small Tafel slope down to 48.8 mV dec⁻¹ and long‐term durability over 80 h. The efficient activity is ascribed to the amorphous nanosheets structure, high electrochemically active surface area, enhanced surface wettability and the synergistic effect of the active metal atoms. This study significantly indicates that CoV−Pi is a promising alternative to replace expensive noble metal‐based catalysts for electrochemical water splitting.