“…Tremendous research efforts have been devoted to the design and development of transition metal‐based substances for water decomposition catalysis, e. g. sulfides, [17,18] carbides, [19] phosphates, [3,20,21] borides, [22] hydroxides, [23–25] metal oxides [26] and so on [27,28] . Well‐known layered double hydroxides (LDHs) such as NiFe‐LDH, [29–31] NiCo‐LDH, [32,33] NiMn‐LDH, [34] NiTi‐LDH, [35] NiV‐LDH [36,37] have also been deemed as “star materials” for many years with impressive catalytical performances due to their large surface area and the adjustable chemical composition in layered structure. Puzzlingly, NiAl LDH as a host material towards water decomposition did not inherit the excellent catalytical ability but with sluggish water‐decomposition kinetics and relatively poor electrocatalytic activity [38] .…”