Electrocatalysts for oxygen reduction reaction (ORR) play a key role in renewable energy technologies including metal-air batteries and fuel cells. Despite tremendous efforts, the development of ORR electrocatalysts with high activity and low cost remains a great challenge. Here, we report the fabrication of well-defined carbon network with honeycomb-like structure as a high-performance catalyst toward ORR, via pyrolysis of bimetallic Co, Zn-zeolitic imidazolate (Co, Zn-ZIF) crystal arrays grown on the surface of layered double hydroxide nanoplatelets (LDHs@Co, Zn-ZIF). The concentration of doped-heteroatoms (N, Co), the graphitic degree as well as the surface porosity of the resulting carbon network can be finely controlled by tuning the Co/Zn molar ratio in the LDHs@Co, Zn-ZIF precursors. The optimal carbon catalyst (CoZn-2) exhibits excellent ORR activity with an onset potential of 0.976V vs. RHE and a limited current density of 5.8mAcm−2, which is superior to commercial Pt/C catalyst. In addition, both an extraordinary long-term stability (∼99.5% current retention over 20,000s) and a strong tolerance against methanol corrosion are also obtained. This work demonstrates an effective strategy to artificially regulate the nanostructure and intrinsic active site of carbon-based ORR electrocatalysts.