In this work, a combination of bottom-up electrochemical deposition and top-down electrochemical etching strategies followed by a subsequent sulfuration treatment was employed to rationally synthesize a nickel sulfide (NiS x) freestanding holey film (FHF). Owing to the holey structure along with the optimal electrochemically active surface area and active sites, the as-prepared NiS x FHF showed an impressive bifunctional electrocatalytic performance toward both oxygen evolution and reduction reactions. The holey and freestanding features provide the NiS x FHF with promising characteristics to be used as an ideal air-breathing cathode in flexible Zn-air batteries (ZABs). As a proof-of-concept, the rationally designed NiS x FHF achieved remarkable rechargeability and flexibility in a ZAB configuration.