Two laboratory analytical methods ? suspended-sediment concentration (SSC) and total suspended solids (TSS) ? are predominantly used to quantify concentrations of suspended solid-phase material in surface waters of the United States. The analytical methods differ. SSC data are produced by measuring the dry weight of all the sediment from a known volume of a water-sediment mixture. TSS data are produced by several methods, most of which entail measuring the dry weight of sediment from a known volume of a subsample of the original. An evaluation of 3,235 paired SSC and TSS data, of which 860 SSC values include percentages of sand-size material, shows bias in the relation between SSC and TSS ?SSC values tend to increase at a greater rate than their corresponding paired TSS values. As sand-size material in samples exceeds about a quarter of the sediment dry weight, SSC values tend to exceed their corresponding paired TSS values. TSS analyses of three sets of quality-control samples (35 samples) showed unexpectedly small sediment recoveries and relatively large variances in the TSS data. Two quality-control data sets (18 samples) that were analyzed for SSC showed both slightly deficient sediment recoveries, and variances that are characteristic of most other quality-control data compiled as part of the U.S. Geological Survey?s National Sediment Laboratory Quality Assurance Program. The method for determining TSS, which was originally designed for analyses of wastewater samples, is shown to be fundamentally unreliable for the analysis of natural-water samples. In contrast, the method for determining SSC produces relatively reliable results for samples of natural water, regardless of the amount or percentage of sand-size material in the samples. SSC and TSS data collected from natural water are not comparable and should not be used interchangeably. The accuracy and comparability of suspended solid-phase concentrations of the Nation?s natural waters would be greatly enhanced if all these data were produced by the SSC analytical method.