Sediments mobilized by interrill erosion are often highly enriched in soil organic carbon (SOC) in comparison to source soils. This selectivity may lead to the preferential mobilization of SOC with specific properties, e.g., SOC that is especially susceptible to decomposition. This may then have important implications with respect to the role of soil erosion in the global carbon cycle. We addressed this issue by investigating the behavior of different SOC components in field rainfall simulation experiments on arable fields in loess-derived soils. We characterized the mobilization of mineral-bound organic carbon (MOC) and particulate organic carbon (POC) by interrill erosion using size fractionation and we used the C:N ratio as a tracer variable to determine the composition of the SOC in eroded sediments. MOC was found to be preferentially mobilized by interrill erosion in comparison to POC. The enrichment ratio (i.e., the ratio of the concentration of a soil constituent in the eroded sediment to its concentration in the original soil) of MOC decreased with increasing sediment concentration. The enrichment ratio of POC displayed a similar pattern to that of MOC but enrichment was less pronounced. Furthermore, sediments were found to be enriched in fine POC while they were impoverished with respect to coarse POC. The selective MOC mobilization together with the dominance of MOC in the total SOC pool in the soil explained the dominance of MOC in interrill eroded sediment. The fact that it is mainly MOC that is mobilized by interrill erosion implies that the SOC in the interrill eroded sediments is on average at least as recalcitrant than that in the source soils which may have important implications for the fate of the mobilized SOC. In order to understand the role of soil erosion in C cycling, MOC and POC need to be considered separately not only because they are chemically different but also because of their different behaviors with respect to geomorphic processes.