| Summary: | Abstract Metal–organic frameworks (MOFs) are recognized as promising electrocatalysts for the oxygen evolution reaction (OER) because of their permanent porosity and rich architectural diversity; however, ionic MOFs enabling fast ions exchange during OER are rarely explored. Here, an ionic MOF (Ni‐btz) constructed with an azolate ligand is selected, and continuous 3D bimetallic MOF (NiFe‐btz) films deriving from high‐degree intergrowth of microsized MOFs particles are fabricated. The as‐prepared NiFe‐btz/NF‐OH electrode exhibits excellent OER performance with a low overpotential of 239 mV at 10 mA cm−2 under alkaline condition. The OER charge transfer process and bimetallic coupling effect in ionic NiFe‐btz are probed by density functional theory calculations and confirmed via X‐ray photoelectron spectroscopy and in situ Raman measurements. The partial density of states of NiFe‐btz indicates that the main contribution for electron density around the Fermi level is from Cl ions clarifying the profitable impact of ionic MOF framework. This work systematically demonstrates the relationship of electronic structure and OER activity in ionic, bimetallic MOFs and expands the scope of 3D MOF films for efficient OER.
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