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All-inorganic halide perovskite single crystals have attracted significant attention in optoelectronic fields on account of their outstanding optoelectronic properties. Photodetectors (PDs) based on CsPbBr 3 single crystal exhibit high responsivity (R) and external quantum efficiency (EQE) due to the direct optical band gap, large optical absorption throughout the visible spectrum range, and long-term stability. Herein, we prepared the centimetersize CsPbBr 3 perovskite single crystal and utilized Zr ion implantation to modify the photoelectric properties of single crystals. The optical band gap of the CsPbBr 3 single crystal decreases from 2.24 to 2.12 eV, and the absorption intensity increases after Zr ion implantation. The R and EQE of the CsPbBr 3 single crystal photodetector modified by Zr ion implantation are 1.0 A W −1 and 294%, respectively, with a light intensity of 3.8 mW cm −2 and a 5 V bias under 425 nm illumination, which are ten times larger than that of the pristine devices. Meanwhile, the first-principles calculation results show that the introduction of Zr ions decreases the band gap and that the Zr 4d orbit contributes to the conduction band minimum (CBM), which facilitates carrier transport in Zr ion implanted CsPbBr 3 single crystals. The results show that Zr ion implantation is an effective strategy to improve the performance of the CsPbBr 3 single-crystal-based PDs.

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