•Multiple tracers were employed to identify the sources of eroded OM in sediments.•Gully banks were the main contributing sources to eroded bulk OM at multiple scales.•Sediment bulk OM mainly sourced from the region with light erosion intensity.•Biological production of OM impacted on the dynamics of water-extractable OM. Erosion is a fundamental phenomenon that governs the biogeochemical cycle of carbon (C) in the Earth system. Understanding the fate of eroded C at the watershed scale thus provides essential guidance for balancing the C budget and evaluating soil management strategies. In this study, we collected a total of 229 topsoils of source materials land use types (forests, grassland, cropland, orchard, and fallow) and gully bank and a total of 56 surface sediment samples main river channel (18) and three tributaries (38) with different erosion intensity. Multiple tracers (C and nitrogen (N) isotopes, molecular n-alkane biomarker, and spectroscopic indices) applied widely were then analyzed to determine relative source contributions to eroded organic matter (OM) (including bulk OM and water-extractable OM) in sediments at a broader watershed on the Loess Plateau of China. The results from an isotopic mixing model analysis showed that gully bank was the primary contributor of bulk OM in sediments, accounting for mean probability estimate (MPE) 55.3%, followed by “grassland” (MPE 21.0%), “cropland” (MPE 14.4%), and “forests” (MPE 9.3%). The contributions of grassland and cropland showed an increasing trend from upstream to downstream sections of the studied watershed. The contribution of forests was found higher in upstream than those of midstream and downstream. Along with previous evidences, our results show that erosion intensity mainly affects the proportion of C source, where gully bank was found as the highest contributor in three associated catchments, especially in region with light erosion intensity. We further demonstrated that the sediment bulk OM deposited was mainly derived from the region with light erosion intensity at the broader watershed scale. Moreover, results of n-alkane ratios and spectroscopic indices also implied that biological production of OM other than terrestrial sources (i.e., soil OM) might play a critical role in source contribution of water-extractable OM in sediments of main river channel.