| Summary: | Semiconductor photocatalysis attracts widespread interest in water splitting, CO2 reduction, and N2 fixation. N2 reduction to NH3 is essential to the chemical industry and to the Earth's nitrogen cycle. Industrially, NH3 is synthesized by the Haber–Bosch process under extreme conditions (400–500 °C, 200–250 bar), stimulating research into the development of sustainable technologies for NH3 production. Herein, this study demonstrates that ultrathin layered‐double‐hydroxide (LDH) photocatalysts, in particular CuCr‐LDH nanosheets, possess remarkable photocatalytic activity for the photoreduction of N2 to NH3 in water at 25 °C under visible‐light irradiation. The excellent activity can be attributed to the severely distorted structure and compressive strain in the LDH nanosheets, which significantly enhances N2 chemisorption and thereby promotes NH3 formation.
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