Concentrations of carbonaceous particles in atmospheric dustfall particles in Huangshi, an industrial city in central China, were determined using a thermal-optical reflectance method. The black carbon (BC) contents in ninety-five dustfall samples ranged from 4.3 to 64.9 g kg–1 with an average of 17.0 g kg–1. These values were higher than those in world background soils and demonstrated serious contamination of the environment in this city. Overall, BC accounted for 17.6–71.3% (mean: 42.0%) of the organic carbon (OC), and BC and OC were positively correlated (r2 = 0.90). Average char and soot contents were 8.01 g kg–1 and 8.65 g kg–1, respectively, and char/soot ratios ranged from 0.28 to 1.97 with an average of 1.01. All the measured carbonaceous species positively correlated with each another, suggesting their common sources. BC, char, and soot showed large spatial distribution variability, with high levels of BC adjacent to the presumed emission sources, such as a power plant and railway line. Analyses of BC/OC and char/soot ratios indicate major impacts from fossil fuel combustion, especially motor vehicle emissions and coal combustion. Industrial dusts related to coal use appear to be the major contributor to BC in dustfall, and this is likely related to the extensive industrial activities in the city, including metal smelting.