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Cost-effective highly efficient and stable catalysts and alkali-resistant anion exchange membranes (AEMs) are critical for practical applications of anion exchange membrane water electrolyzers (AEMWEs). Here, bifunctional non-precious FeCoNiCuMo high entropy alloys (HEAs), electrochemically deposited on nickel mesh as an anode (FeCoNiCuMo/NM) and on carbon paper as a cathode (FeCoNiCuMo/CP), together with a NiFe layered double hydroxide (LDH) loaded AEM (AEM/LDH), were developed for high performance AEMWEs. The AEMWE thus fabricated delivered an ultrahigh current density of 1777 mA cm−2 at 2 V and exhibited remarkable stability with a less than 0.1% cell voltage increase after a 100-hour operation at 100 mA cm−2 at 50 °C, largely outperforming those of the precious metal based AEMWE, composed of IrO 2 /NM as the anode and Pt/C/CP as the cathode, 1231 mA cm−2@2 V and 4.57% increase in cell voltages. Composition of the alkali-resistant, hydrophilic, and water electrolysis active NiFe LDH into the AEM improved not only the electrolyte uptake and operational stability, but also the efficiency of the AEMWE, with a 10% boost in current density achieved at 2 V and a reduction in cell voltage increases from 2.94% to 0.0951%. The present development demonstrates the practicality of AEMWEs toward green hydrogen production. [Display omitted] • Bifunctional non-precious FeCoNiCuMo high entropy alloy catalysts for AEMWE. • Highly alkali-resistant NiFe LDH loaded anion exchange membranes for AEMWE. • Achieve ultrahigh current density of 1777 mA cm−2 at 2 V. • Less than 0.1% cell voltage increase after 100-hour operation at 100 mA cm−2. [ABSTRACT FROM AUTHOR]