η) are thus needed to drive these reactions. RuO 2 /IrO 2 and Pt-based materials are currently considered as the state-ofthe-art electrocatalysts for OER in alkaline conditions and HER in acidic conditions, respectively. But their high cost and scarcity hinder their practical uses. Another important aspect, researchers expect that electrocatalysts are able to work in the same alkaline media for both OER and HER processes to achieve superior FWS performances. Earth-abundant elementbased electrocatalysts, [6][7][8][9][10][11][12][13][14][15][16][17][18][19][20] such as transition-metal oxides, carbides, sulfides, phosphides, and graphdiyne, are promising alternatives to precious electrocatalysts. However, most of them are effective for OER, but very inactive to HER in alkaline condition and vice versa. We can find that there is still a lack of low cost, high efficiency bifunctional OER/HER electrocatalysts in practical applications.Transition metal carbonate hydroxides (TMCHs) are a class of layered materials, which comprised of positive-charged cations and intercalated anions in the interlayer region. [15][16][17][18] Such structure has rich redox properties and high accessibility to electrolyte, providing a very interesting possibility in developing electrocatalysts with efficient electrocatalytic activities. However, because of its low conductivity, only very limited focus has been put on the electrocatalytic behavior of TMCHs. For example, cobalt carbonate hydroxide microspheres required 466 mV, [15] cobalt carbonate hydroxide on carbon black required 509 mV, [16] and cobalt carbonate hydroxide superstructures on carbon paper needed 240 mV [17] to deliver 10 mA cm −2 , respectively. Obviously, the electrocatalytic activities of the reported TMCHs are still far from practical applications. Making the TMCHs with excellent electrocatalytic activities and stabilities is therefore of great significance.The first-row (3d) TMs (e.g., Co and Fe) are promising candidates for precious catalysts. For TM hydroxides, the cations on the surface are considered to be the active sites during the catalytic processes. The introduction of dopants or changing of the M 2+ /M 3+ molar ratios have been reported to effectively tune the electronic structure and lead to optimal adsorption energies toward higher electrocatalytic activity. [4,19,20] Recently, Zhang et al. reported that the OH adsorption energy was either too weak on CoOOH(01-12) surface or too strong on FeOOH(010) surface. [4] After being doped with Fe, the OH adsorption energy was reduced by ≈50% compared with the unary CoOOH(01-12)The controllable synthesis of single-crystallized iron-cobalt carbonate hydroxide nanosheets array on 3D conductive Ni foam (FCCH/NF) as a monolithic oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) bifunctional electrocatalyst for full water splitting is described. The results demonstrate that the incorporation of Fe can effectively tune the morphology, composition, electronic structure, and electrochemical active surface ...