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[Display omitted] Designing heterojunction catalysts with energy effects at the interface, particularly combining the surface structure advantages of super-hydrophilic interfaces with the high activity advantages of bimetal synergistic optimisation, is the key to developing economical and efficient industrial electrocatalytic water-splitting catalysts. In this study, a coupled nanoflower-like NiFe(OH) x /(Ni, Fe)Se heterostructure catalyst supported on Ni foam (NF) (NFSe@NFOH/NF) was designed and successfully prepared using hydrothermal and electrodeposition strategies. Owing to the electron interaction at the heterogeneous amorphous (NFOH)/crystalline (NFSe) interface and the bimetallic synergistic effect of Ni and Fe, the prepared NFSe@NFOH/NF exhibited excellent and stable oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) catalytic properties, with low overpotentials of 214/276 mV at 100 mA⋅cm−2 and 262/340 mV at 500 mA⋅cm−2. The assembled water electrolyser comprising NFSe@NFOH/NF || NFSe@NFOH/NF needed only small voltages of 1.73 and 1.85 V to yield current densities of 100 and 500 mA⋅cm−2, respectively. This study offers an innovative design idea for the rational adoption of interface engineering and amorphous–crystalline engineering techniques to construct catalysts with excellent catalytic activity and stability for electrocatalytic overall water splitting (EOWS) at a high current density, which further facilitates the advancement of sustainable energy technology in the future. [ABSTRACT FROM AUTHOR]