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Circularly polarized light (CPL) detection is of great significance in various applications such as drug identification, sensing and imaging. Atomically precise chiral metal nanoclusters with intense circular dichroism (CD) signals are promising candidates for CPL detection, which can further facilitate device miniaturization and integration. Herein, we report the preparation of a pair of optically active chiral silver nanoclusters [Ag7(R/S‐DMA)2(dpppy)3] (BF4)3 (R/S‐Ag7) for direct CPL detection. The crystal structure and molecular formula of R/S‐Ag7 clusters are confirmed by single‐crystal X‐ray diffraction and high‐resolution mass spectrometry. R/S‐Ag7 clusters exhibit strong CD spectra and CPL both in solution and solid states. When used as the photoactive materials in photodetectors, R/S‐Ag7 enables effective discrimination between left‐handed circularly polarized and right‐handed circularly polarized light at 520 nm with short response time, high responsivity and considerable discrimination ratio. This study is the first report on using atomically precise chiral metal nanoclusters for CPL detection. [ABSTRACT FROM AUTHOR]