Controlled anion-mixing in halide perovskites has been shown to be an effective route to precisely tuning optoelectronic properties, in order to achieve efficient photo- voltaic, light emission and radiation detection devices. However, an atomistic under- standing behind the precise mechanism impacting the performances of mixed halide perovskite devices, particularly as a radiation detector, is still missing. Combining high-level computational methods and multiple experiments, here we systematically investigate the effect of chlorine (Cl) incorporation on the optical and electronic prop- erties, structural stability, ion-migration as well as the γ-ray radiation detection ability of MAPbBr 3-x Cl x . We observe that precise halide mixing suppresses bromide ion mi- gration and consequently reduces the dark current by close to a factor of two, which significantly improves the resistance of the mixed-anion devices. Furthermore, reduced carrier effective masses and mostly unchanged exciton binding energies indicate en- hanced charge carrier transport for these perovskite alloys. At the atomistic level, modifications to ion migration and charge carrier transport properties improve elec- tronic properties and predominantly contribute to the better response and resolution in high-energy γ-ray detection with MAPbBr 3-x Cl x , as compared to MAPbBr 3 . This study provides a systematic approach to enhance the high-energy radiation detection ability of MAPbBr 3-x Cl x -based devices by understanding the atomistic properties un- derpinning performance.