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Nitrogen (N) and phosphorus (P) losses from agricultural soils have been identified as a major contributor to declining surface water quality. Field experiments were conducted to evaluate the effects of cash crops on surface runoff N and P concentrations and loadings in the north part of Huaihe River Basin, China. The treatments comprised three cropping systems including soybean, cotton, and corn, with a bare plot as control. Runoff volume, sediment yield, runoff N and P loadings were significantly affected by the cash cropping system, in the order of bare plot> corn plot> cotton plot> soybean plot. The variation of runoff and sediment yield from different cash cropping systems correlated to the Leaf Area Index (LAI). The factors affecting the loadings of N and P were also closely related to LAI and surface runoff volume. Dissolved N and dissolved P were the main forms of N and P losses for cotton and soybean plots, whereas the particulate N and dissolved P were the main forms of N and P losses for corn plot. Soybean and cotton production can be the cropping systems that reduce the N and P surface losses during the peak-flow production period, if economically feasible.