AbstractLead‐free single crystal perovskite materials exhibit impressive characteristics, such as high carrier mobility, low trap density, and long diffusion length. Herein, the high‐performance blue light photodetectors are reported based on lead‐free all‐inorganic Cs3Sb2Br9 perovskite single crystals. These millimeter‐sized Cs3Sb2Br9 single crystals have small thermal activation energy of 56.8 meV estimated by temperature‐dependent photoluminescence study. There is no obvious structural phase transition of the as‐obtained Cs3Sb2Br9 single crystals since no Raman peak shift is observed with temperature increasing from 80 to 300 K. The as‐constructed high quality Cs3Sb2Br9 single crystals photodetectors have an excellent performance of a responsivity of 2.29 A W−1, a sharp detectivity of 3.77 × 1012 Jones, and an external quantum efficiency (EQE) peak of 1.8 × 103%. Moreover, the photodetectors exhibit a fast response time (<0.2 ms) and the full width at half maximum (FWHM) of the sharp EQE peak is as narrow as 15 nm. This work provides a promising strategy in the design of lead‐free, stable, and high‐performance perovskites for photodetector devices.