The electrochemical converting CO 2 into valuable fuels or chemicals and water splitting to produce hydrogen have become effective strategies to solve the energy crisis. [2] However, both the oxygen evolution reaction (OER) of water splitting to produce hydrogen and the cathode of electrochemical carbon dioxide reduction reaction (CO 2 RR) are multielectron transfer processes, which face a high reaction energy barrier. [3] Thus, it is necessary to develop a highly efficient catalyst to reduce the overpotential of OER and improve the activity and selectivity of CO 2 RR. [4] Currently, most of the catalysts for OER and CO 2 RR are noble metal-based catalysts, such as RuO 2 (for OER) and Au (for CO 2 RR). [5] However, noble metals have a low storage capacity on earth and high cost, so their widespread use on scale-up deployment is severely restricted. [6] Now it is critical to design low-cost and earth-abundant catalysts to replace the noble metal-based electrocatalysts. [7] Recently, layered double hydroxides (LDH) as one of the non-noble metals have been found as efficient OER catalysts because of their unique 2D lamellar structures. [8] For example, NiFe-LDH, [9] CoFe-LDH, [10] and NiV-LDH [11] are well-proven as excellent OER electrocatalysts under alkaline conditions. Unfortunately, the widespread application of LDH in OER is still unsatisfactory, mainly caused by the following two reasons. On the one hand, because the active sites of Bulk LDH are not fully exposed. [12] To solve this problem, liquid-exfoliation [13] and dry-exfoliation [10] of Bulk LDH have been systematically developed to expose more active sits. On the other hand, LDH has a low electron transfer efficiency in catalytic process. Combining LDH with conductive materials is a very effective way to improve the conductivity of LDH, such as carbon nanotubes (CNT), [14] graphene, [13,15] carbon quantum dots, [12] and other alkali corrosion-resistant carbon materials. [16] Over the past few years, researchers have also prepared various catalysts for CO 2 RR, such as non-metal elements (e. g., N, P, and S) doped carbon materials, [17] metal alloys, [18] and mental anchored on N doped carbon support (M-N-C). [19] Among them, the M-N-C has sparked considerable interest as CO 2 RR electrocatalysts,