Abstract: | Herein in we report the unprecedented catalytic activity of an iron‐based oxygen‐deficient perovskite for the oxygen‐evolution reaction (OER). The systematic trends in OER activity as a function of composition, defect‐order, and electrical conductivity have been demonstrated, leading to a methodical increase in OER catalytic activity: Ca2Fe2O6?δ<CaSrFe2O6?δ<Sr2Fe2O6?δ. Sr2Fe2O6?δ also has the highest electrical conductivity and a unique type of defect‐order. In conventional experiments using glassy carbon electrode, Sr2Fe2O6?δ shows better OER activity than the current state of the art catalysts, Ba0.5Sr0.5Co0.8Fe0.2O3?δ and RuO2. It also offers a high intrinsic electrical conductivity, which allows it to act as a catalyst without the need for glassy carbon electrode or carbon powder. Pure disks of this material exhibit an outstanding activity for OER, without any additives or need for electrode preparation. |