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Abstract According to the 2018 National Air Pollutant Emissions Inventory (NEI), air pollutant emissions in the Republic of Korea comprised 808,801 tons of CO, 1,153,265 tons of NOX, 300,979 tons of SOX, 617,481 tons of TSP, 232,993 tons of PM10, 98,388 tons of PM2.5, 15,562 tons of black carbon (BC), 1,035,636 tons of VOCs, and 315,975 tons of NH3. As for national emission contributions to primary PM2.5 and PM precursors (NOX, SOX, VOCs, and NH3), major source categories were the road sector for NOX, the industry sector for SOX and PM2.5, and the everyday activities and others sector for VOCs and NH3. In the case of emissions by region, the largest amount of NOX was emitted from the Seoul Metropolitan Areas (SMA; Seoul, Incheon, and Gyeonggi-do, hereafter SMA) and the largest amounts of SOX, PM2.5, VOCs, and NH3 were from the Yeongnam region. A 3D chemical transport modeling system was used to examine the uncertainty of the national air pollutant emissions based on the National Emission and Air Quality Assessment System (NEAS). Air quality was simulated using CAPSS 2018, and the simulation data were compared with observed concentrations to examine the uncertainties of the current emissions. These data show that emissions from five si (cities) (Pohang, Yeosu, Gwangyang, Dangjin, and Ulsan) need to be improved. Most of all, it is necessary to examine the emissions from places of business that use anthracite, which is the major PM2.5 emission source, as fuel in these areas.