In-stream suspended sediment and siltation and downstream sedimentation are common problems in surface waters throughout the United States. The most effective way to improve surface waters impaired by sediments is to reduce the contributions from human activities rather than try to reduce loadings from natural sources. Total suspended sediment/solids (TSS) concentration data were obtained from 964 streams in the Great Lakes, Ohio, Upper Mississippi, and Souris-Red-Rainy River Basins from 1951 to 2002. These data were used to estimate median concentrations, loads, yields, and volumetrically (flow) weighted (VW) concentrations where streamflow data were available. SPAtial Regression-Tree Analysis (SPARTA) was applied to land-use-adjusted (residualized) TSS data and environmental-characteristic data to determine the natural factors that best described the distribution of median and VW TSS concentrations and yields and to delineate zones with similar natural factors affecting TSS, enabling reference or natural concentrations and yields to be estimated. Soil properties (clay and organic-matter content, erodibility, and permeability), basin slope, and land use (percentage of agriculture) were the factors most strongly related to the distribution of median and VW TSS concentrations. TSS yields were most strongly related to amount of precipitation and the resulting runoff, and secondarily to the factors related to high TSS concentrations. Reference median TSS concentrations ranged from 5 to 26 milligrams per liter (mg/L), reference median annual VW TSS concentrations ranged from 10 to 168 mg/L, and reference TSS yields ranged from about 980 to 90,000 kilograms per square kilometer per year. Independent streams (streams with no overlapping drainage areas) with TSS data were ranked by how much their water quality exceeded reference concentrations and yields. Most streams exceeding reference conditions were in the central part of the study area, where agricultural activities are the most intensive; however, other sites exceeding reference conditions were identified outside of this area. Whether concentrations or yields should be considered in guiding rehabilitation efforts depends on whether in-stream or downstream effects are more important. Although this study attempted to obtain all available water-quality data for the study area, any actual prioritization of sites for remediation would need to rely on more extensive data collection or numerical models that can accurately simulate the effects of various human activities in a range of environmental settings.