This study investigates the most efficient methods for mitigating radiation exposure to residents of rural settlements in five south-west districts of Bryansk Oblast, Russia. A database has been created utilizing modern decision support systems (ReSCA and GISDSS). It contains characteristics of 71 rural settlements, agricultural ecosystems, and forests in the most radioactively contaminated territories of Bryansk Oblast. The authors conducted an assessment to determine the radiological and economic effectiveness of seven technologies aimed at reducing both internal and external exposure for residents who were exposed to a total dose exceeding 1 mSv/year. A list of the most effective measures for each settlement was determined, taking into consideration radiological indicators, cost, and social acceptability of technologies. The application of ferrocene to cattle and the surface improvement of pasture lands in the settlement area have been identified as the most effective measures. The efficiency of radical improvement of hayfields and pastures has significantly decreased since the early 2000s due to the high implementation costs. It has been observed that in ten areas, implementing all efficient remediation technologies will not guarantee a decrease in the overall radiation exposure for the public to a level below 1 mSv/year. Simultaneously, the reduction factor for the total radiation dose experienced by residents in the most vulnerable settlements will be increased by 1.7-2.2 times. The results obtained are crucial for prioritizing further remediation of settlements in south-west Bryansk Oblast and restoring hem to normal living conditions in relation to radiation exposure.