Bi-based inorganic perovskites have attracted great attention in optoelectronics, as they feature similar photoelectric properties but have high stability and lead-free merits. Unfortunately, due to the high exciton binding energy and small Bohr radius, their photodetection performance still largely lags behind that of Pb-based counterparts. Herein, using a vapor-phase chloride ion-substitution strategy, Cs3Bi2Br9 photodetectors (PDs) with gradient energy band alignment were delicately modulated, contributing to a high carrier separation/collection efficiency. The optimized Bi-based perovskite ACCT (Al2O3/Cs3Bi2Br9/Cs3Bi2ClxBr9-x/TiO2) PDs exhibit outstanding performance, the ON/OFF ratio and linear dynamic range (LDR) are significantly improved by 20 and 2.6 times, respectively. Significantly, we further demonstrate the high-SNR (signal-to-noise ratio) UV imaging based on the optimized device, which shows 21.887 dB higher than that of the pristine device. Finally, the vapor-phase anionexchange modified perovskite PDs show long-term stability and high UV resistance. Vapor-phase ion-substitution is a promising approach for the synergistic effect of matched energy band alignment and interface passivation, which can be applied to other perovskite-based optoelectronic devices.