Current theories of land degradation assume that shifts in vegetation communities result in changes to the rates and patterns of water and sediment movement, which are vectors of nutrient redistribution. This nutrient redistribution is hypothesized to reinforce, through positive feedbacks, progressive vegetation changes toward a more degraded ecosystem. A key component of this theory, which is currently poorly resolved, is the relative role of runoff and erosion in driving nutrient fluxes from different vegetation types. We address this gap through a series of field-based, rainfall-simulation experiments designed to explore plant-level dynamics of runoff- and erosion-driven nutrient fluxes of N, P and K species. Our results highlight important linkages between physical and biogeochemical processes that are controlled by plant structure. We found that: 1) the magnitude of sediment-bound nutrient export is determined by the grain-size distribution of the eroded sediment and the total sediment yield; 2) the partitioning of nutrients in dissolved and sediment-bound form is determined by the availability and concentration of different nutrient species in the soil or rainfall; 3) these processes varied according to vegetation type and resulted in stark differences between degrading and invading plant communities. Specifically, we observed that grassland areas consistently exported the highest yields of sediment-bound N, P and K despite producing similar erosion rates to shrub and intershrub areas. Our results have implications for better understanding how grassland areas are being replaced by shrubs and provide insights into the mechanisms of continuing land degradation in drylands.