Dustfall samples from the western Chinese Loess Plateau (CLP) were collected from 2013 to 2016 at Jiuzhoutai for dustfall variation analysis. Results showed that the seasonal dustfall variations were non-significant in the region, indicating dustfall sources with inconsistent patterns largely contributed to the modern loess formation. The average rate of loess accumulation was approximately 0.34 mm/year, which is much higher compared to the other periods of the Holocene. In addition, the lack of regular patterns of dustfall contents in the coarse fraction (> 50 μm in diameter) indicates a proximal source with crustal origins, which is a dominant source for the modern loess. From 2013 to 2016, the dustfall from crustal origins increased by approximately 19%, and among those collected dustfall, approximately 24% came from pollutants, indicating that anthropogenic activities such as industrial pollutants and vehicle emissions played an important role in modern loess accumulation.