The problem in d‐band center modulation of transition metal‐based catalysts for the rate‐determining steps of oxygen conversion is an obstacle to boost the electrocatalytic activity by accelerating proton coupling. Herein, the Co doping to FeP is adopted to modify the d‐band center of Fe. Optimized Fe sites accelerate the proton coupling of oxygen reduction reaction (ORR) on N‐doped wood‐derived carbon through promoting water dissociation. In situ generated Fe sites optimize the adsorption of oxygen‐related intermediates of oxygen evolution reaction (OER) on CoFeP NPs. Superior catalytic activity toward ORR (half‐wave potential of 0.88 V) and OER (overpotential of 300 mV at 10 mA cm−2) express an unprecedented level in carbon‐based transition metal‐phosphide catalysts. The liquid zinc–air battery presents an outstanding cycling stability of 800 h (2400 cycles). This research offers a newfangled perception on designing highly efficient carbon‐based bifunctional catalysts for ORR and OER.