Carbon monoxide (CO) is a key tracer of anthropogenic pollution, and it indirectly affects climate change. Anmyeon-do (AMY, 36.54° N, 126.33° E), a World Meteorological Organization/Global Atmosphere Watch Program (WMO/GAW) regional background station in Korea, provides continuous observations of CO mole fractions at the surface and vertical profiles within 0.5–9 km that are also collected by aircraft campaigns. The vertical profiles collected in 2019 were analyzed using meteorological parameters such as vertical velocity and boundary layer height (BLH), and a strong relationship was observed among them; however, the vertical distribution, which was influenced by unexpected strong pollution plumes, did not exhibit a strong relationship with vertical velocity and BLH. On November 16, we captured a strong CO signal within the boundary layer and at approximately 2 km above the BLH, where vertical profiles of the aerosol scattering coefficient at 550 nm were simultaneously observed with the same vertical structure. To identify the origins and source types of the stratification of the pollution plume for CO and aerosol, we also analyzed surface in situ observations of particle size distributions and reactive gases (NOx, O3, and SO2) as well as the column averaged dry-air mole fraction of carbon monoxide (XCO) and measurements of aerosol optical depth obtained from the tropospheric monitoring instrument (TROPOMI) and moderate resolution imaging spectroradiometer (MODIS) satellite, respectively. The high CO event within the BLH, including observations at the surface site, was attributed to domestic burning sources. Convective uplifting of industrial fossil fuel emissions from eastern China was responsible for the high CO dry mole fraction in the low free troposphere (FT) and the elevated aerosol scattering coefficient. Statistical analyses of one-year surface in situ observations of CO reveal that CO-emission sources from eastern China contributed to extremely high CO spikes (≥80th percentile of CO or ≥ 350 ppb, approximately) in 2019. Therefore, we concluded that emissions from eastern China have a potentially leading role in the observed high pollution events at the surface and the lower FT over the AMY station in 2019. The increase in ground temperature, with the acceleration of the global warming process, can intensify the convective uplifting of pollution plumes from emission source regions to FT over East Asian regions. In addition, such an occurrence of the stratification of the atmospheric pollution plume in the troposphere should be considered in future studies on radiative forcing to improve air-quality forecasting in this region.