Tropospheric ozone (O3) and fine particles (PM2.5) come from both local and regional emissions sources. Due to the nonlinearity in the response of O3 and PM2.5 to their precursors, contributions from multiregional sources are challenging to quantify. Here we developed an updated extended response surface modeling technique (ERSMv2.0) to address this challenge. Multiregional contributions were estimated as the sum of three components: (1) the impacts of local chemistry on the formation of the pollutant associated with the change in its precursor levels at the receptor region; (2) regional transport of the pollutant from the source region to the receptor region; and (3) interregional effects among multiple regions, representing the impacts on the contribution from one source region by other source regions. Three components were quantified individually in the case study of Beijing-Tianjin-Hebei using the ERSMv2.0 model. For PM2.5 in most cases, the contribution from local chemistry (i.e., component 1) is greater than the contribution from regional transport (i.e., component 2). However, regional transport is more important for O3. For both O3 and PM2.5, the contribution from regional sources increases during high-pollution episodes, suggesting the importance of joint controls on regional sources for reducing the heavy air pollution.