This data release contains total dissolved solids (TDS) concentrations and specific conductance (SC) measurements collected at surface-water monitoring locations and groundwater monitoring wells within the Upper Colorado River Basin (UCRB) between 1894 and 2022. Discrete TDS and SC results were obtained from the Water Quality Portal (WQP). Continuous SC monitoring results were obtained from the USGS National Water Information System (NWIS). The data set includes 127,294 TDS results that were collected at 12,339 sites between 1900 and 2022, and 705,918 SC results that were collected at 19,630 sites between 1894 and 2022. The SC results represented 244,784 discrete measurements at 19,625 sites and 461,134 mean daily values from continuous monitoring at 193 sites. The data retrieved from the WQP were harmonized to create a standardized and readily usable dataset. The harmonization process included the synthesis of parameter names and fractions, the reconciliation of remarks and other data qualifiers, the resolution of duplicate records, and basic checks of the data quality. The harmonized results at 230 sites were selected for additional data processing because those sites were potential calibration targets for TDS watershed modeling for the UCRB using the USGS Spatially Referenced Regression on Watershed attributes (SPARROW) model. The 230 sites met the minimum criteria for the number and seasonal distribution of samples, the length of the sampling period, and the amount of overlap with the streamflow record at a nearby gage. The measured TDS concentrations at those sites were supplemented with estimated TDS concentrations that were determined from relations between measured TDS and SC results within the UCRB. A site-specific regression of TDS on SC was used to estimate TDS from SC at 143 sites, while a regional conversion factor between TDS and SC was used to estimate TDS from SC at 87 sites. The final TDS data for the 230 sites included 50,003 measured values from the WQP, 378,147 values estimated using the equation from a site-specific regression of TDS on SC (with 350,840 based on mean daily SC values), and 30,880 values estimated using a regional median ratio between TDS and SC.