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Nickel is a promising candidate as an alternative to ruthenium for an ammonia decomposition catalyst. However, the performance of Ni‐based catalysts for ammonia decomposition is still not sufficient to achieve a good hydrogen production rate under low‐temperature because the weak nitrogen affinity of Ni reduces the frequency of the ammonia decomposition reaction. Here, it is reported that Ni supported on barium titanium oxynitride (Ni/h‐BaTiO3−xNy) with a hexagonal structure acts as a highly active and water‐durable catalyst for ammonia decomposition. The operation temperature is reduced by over 140 °C when N3− ions are substituted onto the O2− sites of the BaTiO3 lattice, and the Ni/h‐BaTiO3−xNy catalyst significantly outperforms conventional oxide‐supported Ni catalysts for ammonia decomposition. Furthermore, the activity of Ni/h‐BaTiO3−xNy remains unchanged after exposure to water. The 15NH3 decomposition reaction and Fourier transform‐infrared spectroscopy (FT‐IR) measurements reveal that lattice nitrogen vacancy sites on h‐BaTiO3−xNy function as the active sites for ammonia decomposition. The ammonia decomposition activity of Ni/h‐BaTiO3−xNy is also higher than that of the Ni/h‐BaTiO3−xHy oxyhydride catalyst, making a contrast to the activity trend in ammonia synthesis. [ABSTRACT FROM AUTHOR]