The spatial and temporal variability in streambed-sediment quality and its relation to historical water quality was assessed to provide guidance for the development of total maximum daily loads and the implementation of best-management practices in the Little Arkansas River Basin, south-central Kansas. Streambed-sediment samples were collected at 26 sites in 2007, sieved to isolate the less than 63-micron fraction (that is, the silt and clay), and analyzed for selected nutrients (total nitrogen and total phosphorus), organic and total carbon, 25 trace elements, and the radionuclides beryllium-7, cesium-137, lead-210, and radium-226. At eight sites, streambed-sediment samples also were collected and analyzed for bacteria. Particulate nitrogen, phosphorus, and organic carbon concentrations in the streambed sediment varied substantially spatially and temporally, and positive correlations among the three constituents were statistically significant. Along the main-stem Little Arkansas River, streambed-sediment concentrations of particulate nitrogen and phosphorus generally were larger at and downstream from Alta Mills, Kansas. The largest particulate nitrogen concentrations were measured in samples collected in the Emma Creek subbasin and may be related to livestock and poultry production. The largest particulate phosphorus concentrations in the basin were measured in samples collected along the main-stem Little Arkansas River downstream from Alta Mills, Kansas. Particulate nitrogen, phosphorus, and organic carbon content in the water and streambed-sediment samples typically decreased as streamflow increased. This inverse relation may be caused by an increased contribution of sediment from channel-bank sources during high flows and (or) increased particle sizes transported by the high flows. Trace element concentrations in the streambed sediment varied from site to site and typically were less than threshold-effects guidelines for possible adverse biological effects. The largest copper, lead, silver, and zinc concentrations, measured for a sample collected from Sand Creek downstream from Newton, Kansas, likely were related to urban sources of contamination. Radionuclide activities and bacterial densities in the streambed sediment varied throughout the basin. Variability in the former may be indicative of subbasin differences in the contribution of sediment from surface-soil and channel-bank sources. Streambed sediment may be useful for reconnaissance purposes to determine sources of particulate nitrogen, phosphorus, organic carbon, and other sediment-associated constituents in the basin. If flow conditions prior to streambed-sediment sampling and during water-quality sampling are considered, it may be possible to use streambed sediment as an indicator of water quality for nitrogen, phosphorus, and organic carbon. Flow conditions affect sediment-associated constituent concentrations in streambed-sediment and water samples, in part, because the sources of sediment (surface soils, channel banks) can vary with flow as can the size of the particles transported.