In recent years, the problem of atmospheric pollution has been concerning in the Beijing–Tianjin–Hebei region, due to the frequent haze. It has become a significant issue to improve regional air quality through appropriate emission reduction measures. In this study, considering the regional atmospheric transmission of air pollutants, the WRF/CALPUFF model (the Weather Research and Forecasting model coupled with the California Puff air quality model) was used to describe the impact of each city’s pollutant emissions on the concentrations of every city. Then, a new optimization model was designed to calculate the maximum allowable emissions of every city. The results showed that NOx and PM_2.5 emissions need to be reduced by 44% and 48%, respectively, in the traditional mitigation scenario (any city’s pollutant emissions are not allowed to increase). However, in the optimized scenario, NOx and PM_2.5 emissions should be reduced by 23% and 46%, respectively, to meet the national secondary standard. The emissions of cities with low transfer coefficients, such as Zhangjiakou, Qinhuangdao, and Chengde, could even be appropriately increased. This means that the optimized scenario could reduce the pressure on emission reduction. Although the optimization results are theoretical and idealistic, this research study provides a new idea for formulating emission mitigation policies in various regions to reduce the impact on the economy.