Considering the intermittency of typical renewable and environment-friendly energy resources, such as wind, tide, and solar energy, it is encouraging to explore all-weather utilization ones. [1] Electrochemical water splitting for hydrogen and oxygen production may overcome the challenge as an ideal sustainable system for the future. [2] Unfortunately, the high activation barriers and sluggish kinetics of hydrogen and oxygen evolution reactions (HER and OER) hindered their further applications. [3] Since HER and OER must be operated in the same electrolyte for overall water splitting, efficient bifunctional electrocatalysts, which can prevent cross-contamination, materials incompatibilities, and possible catalyst poisoning, are attracting everincreasing attentions. [4] Earth-abundant transition metal layered double hydroxides (LDHs) have been recognized as promising electrocatalysts