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Abstract A crucial step toward clean hydrogen (H₂) energy production through water electrolysis is to develop high‐stability catalysts, which can be reliably used at high current densities for a long time. So far, platinum group metals (PGM) and their oxides, for example, Pt and iridium oxide (IrO₂) have been well‐regarded as the criterion for hydrogen and oxygen evolution reactions (HER and OER) electrocatalysts. However, the PGM catalysts usually undergo severe performance decay during the long‐term operation. Herein, the in situ growth of iron phosphosulfate (Fe₂P₂S₆) nanocrystals (NCs) catalysts on carbon paper synthesized by combing chemical vapor deposition with solvent‐thermal treatment is reported to show competitive performance and stability as compared to the state‐of‐the‐art PGM catalysts in a real water electrolyzer. A current density of 370 mA cm⁻²is achieved at 1.8 V when using Fe₂P₂S₆NCs as bifunctional catalysts in an anion exchange membrane water electrolyzer. The Fe₂P₂S₆NCs also show much better stability than the Pt‐IrO₂catalysts at 300 mA cm⁻²for a continuous 24 h test. The surface generated FeOOH on Fe₂P₂S₆is the real active site for OER. These results indicate that the Fe₂P₂S₆NCs potentially can be used to replace PGM catalysts for practical water electrolyzers.