has surpassed 25.5%, [2] and the external quantum efficiency (EQE) of perovskite LEDs has been dramatically boosted to over 20%. [3] However, there exist two main problems with organic lead halide perovskites. First, the toxicity of lead in perovskite has severely restricted its commercialization. Therefore, on the basis of inheriting the excellent performance of lead-based perovskites, it is of great significance to develop nontoxic lead-free halide perovskites for optoelectronic applications. [4] To date, a rapid development has been achieved in the past years, and a large amount of environment-friendly metal cations have been selected to replace Pb 2+ to reduce the toxicity to humans and the environment, including Sn 2+ , Cu + , Bi 3+ , Ge 2+ , and Sb 3+ . [2] Second, the instability to moisture, light and heat, which comes from the intrinsic organic cationic group, limits its practical application. [4] From the application point of view, it is required that the lead-free halide perovskite should exhibit enough stability to the disturbance from external environment. It is proved that reducing the structural dimensions of the perovskite can effectively improve its stability. [5] Consequently, low-dimensional metal halide perovskite analogues at molecular level, which demonstrate good stability and unique photophysical properties, have attracted tremendous attention in the field of optoelectronics. [6] Recently, as an ideal candidate of novel low-dimensional metal halide perovskite analogues, 1D CsCu 2 I 3 has been investigated in many aspects of photodetection field. Highly stable CsCu 2 I 3 single crystal was fabricated as facet-dependent, fast response, and broadband photodetector. [7] Oriented-structured CsCu 2 I 3 film detector achieved high-resolution X-ray imaging. [8] Solution-processed CsCu 2 I 3 nanowires were introduced to construct polarization-sensitive and flexible UV photodetector. [9] High-performance deep UV photodetector was built up based on the CsCu 2 I 3 film. [10] In addition, 1D CsCu 2 I 3 perovskite analogue also shows great potential in the field of LEDs. Highly efficient 1D CsCu 2 I 3 single crystal was emerged as the downconversion phosphors for white-LEDs. [11] Through localized 1D excitonic recombination, a high photoluminescence quantum yield (PLQY) was realized in CsCu 2 I 3 single crystal. [12] However, this typical strong excitonic recombination and short carrier Lead-free ternary copper iodide perovskite analogues demonstrate great potential in photodetector, due to their nontoxity and excellent photophysical properties. However, the fast carrier recombination limits the photoelectric conversion efficiency. Herein, a room-temperature growth strategy with the selected raw ratio is adopted to enhance carrier dynamics. The optimizedgrown CsCu 2 I 3 single crystal exhibits longer carrier lifetime of 157 ns, and its switch ratio and response time are enhanced by 20 000% and 600% compared with those of stoichiometric-grown single crystal, respectively. Furthermore, space-confined meth...