been devoted to various energy storage and conversion systems. [1,2] Metal-air batteries, especially Zn-air batteries (ZABs) have been regarded as a promising energy storage system due to their low-cost, high theoretical specific energy density (1084 Wh kg −1 ), and environmental friendliness. [3][4][5] Nevertheless, the multistep and proton-coupled electron transfer processes of the reversible oxygen reactions lead to sluggish kinetics for oxygen reduction (ORR) and oxygen evolution (OER) at aircathode, which are the bottlenecks of inefficient and unideal lifetime. [6] The current benchmark catalysts for simply ORR or OER are precious-metal-based catalysts (Pt, Ir, RuO 2 , etc.), but their high cost, supply scarcity, and poor bifunctional catalytic characters have greatly restricted their applications in ZABs. [7,8] In response, various transition-based catalysts with high activity and good durability have been explored, such as transition metal oxides, chalcogenides, and metal-heteroatom doped carbon materials. [9][10][11][12][13][14] Despite significant progress, current bifunctional catalysts are still facing the problems of insufficient activity and stability together with poor mass transport properties.Alternatively, metal-nitrogen-carbon (M-N-C) systems comprising the earth abundant transition metals and catalytic active metalN x centers with carbonized ligand have received growing interest due to their low cost and excellent catalytic activities. [15][16][17] Specially, Co-N-C has emerged as ORR catalyst for improvement the overall performance of ZABs. [18,19] Inspired by the excellent OER performance of Co-based catalysts (e.g., cobalt metal and cobalt oxide) and intrinsically electrical conductivity of Co metal, [20,21] so constructing hierarchical structure of Co-N-C contained Co metal maybe an effective way to promote the bifunctional ORR/OER activity. At present, various strategies have been applied to synthesize Co-N-C structures. Traditionally, carbonized the Co-based precursors (such as porphyrins and phthalocyanines) have been developed for several decades to synthesize metal contained N-doped carbon nanostructures, [22,23] but always suffer from large nanoparticles size and ununiformed structures. Hence, much efforts have been devoted to construct Co-N-C-based catalysts with novel morphology and structures, such as core-shell or single-atom dispersed Co-N-C catalysts combined with carbon nanotubes Developing non-precious-metal bifunctional oxygen reduction and evolution reaction (ORR/OER) catalysts is a major task for promoting the reaction efficiency of Zn-air batteries. Co-based catalysts have been regarded as promising ORR and OER catalysts owing to the multivalence characteristic of cobalt element. Herein, the synthesis of Co nanoislands rooted on Co-N-C nanosheets supported by carbon felts (Co/Co-N-C) is reported. Co nanosheets rooted on the carbon felt derived from electrodeposition are applied as the self-template and cobalt source. The synergistic effect of metal Co islands with OER a...