Soil erosion is a key variable in the biogeochemical cycle of carbon (C) on the Earth's surface. However, questions remain about the roles of land use and erosion intensity on the composition, source, and fate of soil C eroded from terrestrial to fluvial systems. In this study, chemical characteristics of eroded water-extractable organic matter (WEOM) in soils and sediments, as well as subsequent source identification, were inferred from UV–Visible absorption and fluorescence excitation emission matrix (EEM)-parallel factor analysis (PARAFAC) in study sites that include land uses and gully banks, experiencing three levels of erosion intensity in a semi-arid region of China. 13C and 15N isotopic signatures along with elemental ratios were also successfully employed to explore the source of bulk soil organic matter (SOM) in sediments. We found a much greater contribution of condensed aromatic structures and hydrophobic fraction of soluble organic compounds in forest soils compared to croplands at eroding sites, where these variables were greater than those of depositional sites. The results from fluorescence analysis in soil materials showed that erosion intensity has a negligible influence on WEOM quality. The EEM-PARAFAC with fluorescence indices indicated that biological production of soil substrates can also play a key role in the dynamics of WEOM induced by soil erosion. Our results from an isotopic mixing model analysis showed that gully bank soil was the primary sources of sedimentary SOM in all regions with different erosion intensities (mean probability estimate (MPE) 100% for the region with light erosion intensity, 36.18% for the region with high erosion intensity, and 99.25% for the region with extremely high erosion intensity). However, orchard and grassland were also the main contributors for the SOM in sediments in regions with high erosion intensity, accounting for MPE 29.93% and 33.89%, respectively. Our findings demonstrate that land use and erosion intensity have significant effect on nature of eroded OM.