摘要： Low-dimensional metal halides at molecular level, which feature strong quantum confinement effects from intrinsic structure, are emerging as ideal candidates in optoelectronic fields. However, developing stable and nontoxic metal halides still remains a great challenge. Herein, for the first time, high-crystalline and highly stable CsCu2I3 single crystal, which is acquired by a low-cost antisolvent vapor assisted method, is successfully developed to construct high-speed (trise/tdecay = 0.19 ms/14.7 ms) and UV-to-visible broadband (300–700 nm) photodetector, outperforming most reported photodetectors based on individual all-inorganic lead-free metal halides. Intriguingly, facet-dependent photoresponse is observed for CsCu2I3 single crystal, whose morphology consists of {010}, {110}, and {021} crystal planes. The on–off ratio of {010} crystal plane is higher than that of {110} crystal plane, mainly owing to lower dark current. Furthermore, photogenerated electrons are localized in twofold chains created by [CuI4] tetrahedra, leading to relatively small effective mass and fast transport mobility along the 1D transport pathway. Anisotropic carrier transport characteristic is related to stronger confinement and higher electron density for {110} crystal planes. This work not only demonstrates the great potential of CsCu2I3 single crystal in high-performance optoelectronics, but also gives insights into 1D electronic structure associated with fast photoresponse and high anisotropy.