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Sediment associated carbon and nitrogen loss under rainfall, an important cause of soil quality degradation and water eutrophication, strongly depends on the intrinsic properties of original soil types. Relative to total loss, the transport behaviors of organic carbon and nitrogen among sediment size classes and response to soil types remain poorly understood. The concentrations of organic carbon (OC) and total nitrogen (TN) in different sediment size classes (>1, 0.25–1, 0.10–0.25, and <0.10 mm) and their contributions to total sediment load during rainfall erosion were determined under field plot rainfall simulation (at 90 mm h−1) on three contrasting soil types (Luvisol, Alisol and Ferralsol) with increased aggregate stability. During rainfall erosion, the concentrations of OC and TN in total and different sized sediments decreased first and then reached a steady state. The variability of OC and TN concentrations (coefficient of variations in 4.2–53.1% and 6.6–41.9%) among sediment size classes decreased from Luvisol to Ferralsol. Compared to original soils, sediments exhibited larger C/N ratios for Luvisol, and smaller values for Alisol, indicating the more selective transport of labile organic matter for weaker aggregated soils. Among sediment size classes, fine particles (<0.10 mm) accounted 69–88% of total OC and TN losses for Luvisol, and decreased to 30–39% for Ferralsol; and the main transport mechanisms of sediment associated OC and TN shifting from suspension-saltation (<0.10 mm) to rolling (>0.25 mm) with increased aggregate stability. Among original soil properties, inorganic cementing agents (including amorphous iron oxides and clay minerals) showed closer relationships with sediment OC and TN losses (|r| = 0.61–0.89, p < 0.001) than organic matter properties (|r| = 0.55–0.87, p < 0.001), further implying the important role of soil aggregate stability across soil types. This study provides an in-depth understanding on soil carbon and nitrogen losses and their divergent characteristics among soil types deserves consideration in the development of erosion model and land management in agricultural systems. • Variability of OC and TN concentrations among sediment sizes decreased from Luvisol to Ferralsol. • Suspension-saltation (<0.10 mm) dominated OC and TN losses for weak aggregated soils. • Contribution of coarse particles by rolling to OC and TN losses increased with aggregate stability. • Runoff rate, iron oxides and sediment size controlled the loss characteristics of OC and TN. [ABSTRACT FROM AUTHOR]