Cobalt and Fe were co-electrodeposited as single crystal, faceted particles onto carbon paper to produce Co/Fe-oxyhydroxide oxygen evolution reaction (OER) catalysts with various Co/Fe ratios. Electron microscopy and Auger electron spectroscopy were used to investigate the morphology and composition of the electrodeposits. Iron content in the deposits increased with increasing Fe concentration in the electrolyte and Fe segregated to the particle surfaces. Electrochemical tests demonstrated that the deposit Co/Fe ratio influences OER activity by altering the electrochemically active surface area (ECSA) and charge transfer resistance. The OER activity increased with increasing Fe content up to ∼65 at% Fe, with a minimum overpotential of 0.33 V at 10 mA cm−2 in 1 M KOH. The fabricated OER catalysts were assembled into a Zn-air battery for discharge-charge cycling tests and showed lower charge potentials compared with bare carbon paper.