Dissolved organic carbon (DOC) constitutes the largest carbon pool in surface waters, with soil being its main source via surface and subsurface runoff. Amendment with organic residues can reduce soil erosion and surface runoff, but little is known how this affects the amount and composition of DOC losses via surface runoff and the associated transfer of nutrients and pollutants. In this study, artificial rainfall experiments were conducted on three pairs of soil runoff plots with contrasting organic matter management. A mixture of grass and wheat straw residues was incorporated into the topsoil of one plot in each pair (OI treatment) but not into the other (control). Artificial rainfall was applied onto both treatments at an intensity of 49.1 mm h−1, and surface runoff samples were collected at designated time steps for analysis of DOC, total dissolved phosphorus (TDP), copper (TDCu) and zinc (TDZn) concentrations, as well as for characterization of DOC by UV–vis absorbance (SUVA254 and E2:E3) and fluorescence spectroscopy (FI) indexes. The organic amendment reduced the loss rates of DOC, TDP, TDCu and TDZn by reducing surface runoff, although increasing the concentrations of DOC, TDP and TDCu. Regardless of the treatment, DOC, TDP and TDCu concentrations were always maximal at the onset of runoff and then continuously decreased after the initial flush. The observed relationships of TDP and TDCu concentrations with DOC indicate that the export of “dissolved” P and Cu primarily occurred in DOC-bound form, while the concentration of TDZn was not correlated with that of DOC. Surface runoff from the amended soils generally contained more hydrophilic and low molecular weight DOC (as indicated by low SUVA254 and high E2:E3 and FI values), particularly at high DOC concentrations. The ratio between TDCu and DOC concentration showed a positive relationship to DOC aromaticity (as indicated by SUVA254 values) in the OI treatment. The results indicate that organic amendment can reduce total rates of dissolved element losses with surface runoff, but attention should also be paid to the composition of lost DOC and the concentrations of DOC-associated solutes.