A flexible air electrode (FAE) with both high oxygen electrocatalytic activity and excellent flexibility is the key to the performance of various flexible devices, such as Zn-air batteries. A facile two-step method, mild acid oxidation followed by air calcination that directly activates commercial carbon cloth (CC) to generate uniform nanoporous and super hydrophilic surface structures with optimized oxygen-rich functional groups and an enhanced surface area, is presented here. Impressively, this two-step activated CC (CC-AC) exhibits superior oxygen electrocatalytic activity and durability, outperforming the oxygen-doped carbon materials reported to date. Especially, CC-AC delivers an oxygen evolution reaction (OER) overpotential of 360 mV at 10 mA cm −2 in 1 m KOH, which is among the best performances of metal-free OER electrocatalysts. The practical application of CC-AC is presented via its use as an FAE in a flexible rechargeable Zn-air battery. The bendable battery achieves a high open circuit voltage of 1.37 V, a remarkable peak power density of 52.3 mW cm −3 at 77.5 mA cm −3 , good cycling performance with a small chargedischarge voltage gap of 0.98 V and high flexibility. This study provides a new approach to the design and construction of high-performance selfsupported metal-free electrodes.

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