Excellent performance and multifunctional electrocatalysts are of great importance for the development of renewable energy. Here, a multifunctional carbon cloth supported cobalt phosphide (CoP@CC) electrocatalyst was synthesized via a simple electrochemical deposition followed by subsequent phosphorization. This self-standing CoP@CC presents superior HER performance in both acid and alkaline media and excellent OER activity in an alkaline environment. When applied as both anode and cathode catalyst to overall water splitting, CoP@CC only required a low cell voltage of 1.68 V to drive a current density of 10 mA cm-2, making this catalyst a potential candidate in industrial application. Moreover, inspired by its satisfying ORR activity, CoP@CC was first used as the air-electrode in zinc-air batteries, which outputted an open-circuit potential of 0.6 V and a power density of ∼30 mW cm-2.