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Bismuth-based halide perovskites have shown great potential for direct X-ray detection, attributable to their nontoxicity and advantages in detection sensitivity and spatial resolution. However, the practical application of such materials still faces the critical challenge of combining both high sensitivity and low detection limits. Here, we report a new type of zero-dimensional (0D) perovskite (HIS)BiI5(1, where HIS2+= histamine) with high sensitivity and a low detection limit. Structurally, the strong N–H···I hydrogen bonds between HIS2+cations and inorganic frameworks enhance the rigidity of the structure and diminish the intermolecular distance between adjacent inorganic [Bi2I10]4–dimers. By virtue of such structural merits, single crystal 1exhibits excellent physical properties perpendicular to both the (001) and (010) faces. Perpendicular to the (010) face, 1exhibited a high electrical resistivity (2.31 × 1011Ω cm) and a large carrier mobility–lifetime product (μτ) (2.81 × 10–4cm2V–1) under X-ray illumination. Benefiting from these superior physical properties, it demonstrates an excellent X-ray detection capability with a sensitivity of approximately 103μC Gyair–1cm–2and a detection limit of 36 nGyairs–1in both directions perpendicular to the (001) and (010) crystal faces. These results provide a promising candidate material for the development of new, lead-free, high-performance X-ray detectors.