It is highly desired to design and develop low-cost and efficient bifunctional electrocatalysts for zinc-air batteries (ZABs). In this communication, we report that Fe-doped CoP nanosheet arrays on nickel foam (Fe0.33-CoP/NF) act as a highly active bifunctional electrocatalyst for both the oxygen reduction reaction and the oxygen evolution reaction in alkaline media. We further demonstrate the use of Fe0.33-CoP/NF as the cathode to construct rechargeable ZABs with superior performance to that of the CoP/NF counterpart. In concentrated alkaline electrolytes, such ZABs exhibit a higher power density of 63 mW cm-2 than that of CoP/NF (23 mW cm-2) with a long cycle life (up to 200 h).