Groundwater quality in the approximately 1,000-square-mile (2,590-square-kilometer) Upper Santa Ana Watershed (USAW) study unit was investigated as part of the Priority Basin Project of the Groundwater Ambient Monitoring and Assessment (GAMA) Program. The study unit is located in southern California in Riverside and San Bernardino Counties. The GAMA Priority Basin Project is being conducted by the California State Water Resources Control Board in collaboration with the U.S. Geological Survey and the Lawrence Livermore National Laboratory. The GAMA USAW study was designed to provide a spatially unbiased assessment of untreated groundwater quality within the primary aquifer systems in the study unit. The primary aquifer systems (hereinafter, primary aquifers) are defined as the perforation interval of wells listed in the California Department of Public Health (CDPH) database for the USAW study unit. The quality of groundwater in shallower or deeper water-bearing zones may differ from that in the primary aquifers; shallower groundwater may be more vulnerable to surficial contamination. The assessment is based on water-quality and ancillary data collected by the U.S. Geological Survey (USGS) from 90 wells during November 2006 through March 2007, and water-quality data from the CDPH database. The status of the current quality of the groundwater resource was assessed based on data from samples analyzed for volatile organic compounds (VOCs), pesticides, and naturally occurring inorganic constituents, such as major ions and trace elements. The status assessment is intended to characterize the quality of groundwater resources within the primary aquifers of the USAW study unit, not the treated drinking water delivered to consumers by water purveyors. Relative-concentrations (sample concentration divided by the health- or aesthetic-based benchmark concentration) were used for evaluating groundwater quality for those constituents that have Federal or California regulatory or non-regulatory benchmarks for drinking-water quality. A relative-concentration greater than (>) 1.0 indicates a concentration above a benchmark, and a relative-concentration less than or equal to (≤) 1.0 indicates a concentration equal to or less than a benchmark. Organic and special-interest constituent relative-concentrations were classified as "high" (> 1.0), "moderate" (0.1 < relative-concentration ≤ 1.0), or "low" (≤ 0.1). Inorganic constituent relative-concentrations were classified as "high" (> 1.0), "moderate" (0.5 < relative-concentration ≤ 1.0), or "low" ( ≤ 0.5). Aquifer-scale proportion was used as the primary metric in the status assessment for evaluating regional-scale groundwater quality. Aquifer-scale proportions are defined as the percentage of the area of the primary aquifer system with concentrations above or below specified thresholds relative to regulatory or aesthetic benchmarks. High aquifer-scale proportion is defined as the percentage of the area of the primary aquifers with a relative-concentration greater than 1.0 for a particular constituent or class of constituents; percentage is based on an areal, rather than a volumetric basis. Moderate and low aquifer-scale proportions were defined as the percentage of the primary aquifers with moderate and low relative-concentrations, respectively. Two statistical approaches—grid-based and spatially weighted—were used to evaluate aquifer-scale proportions for individual constituents and classes of constituents. Grid-based and spatially weighted estimates were comparable in the USAW study unit (within 90-percent confidence intervals). Inorganic constituents with human-health benchmarks had relative-concentrations that were high in 32.9 percent of the primary aquifers, moderate in 29.3 percent, and low in 37.8 percent. The high aquifer-scale proportion of these inorganic constituents primarily reflected high aquifer-scale proportions of nitrate (high relative-concentration in 25.3 percent of the aquifer), although seven other inorganic constituents with human-health benchmarks also were detected at high relative-concentrations in some percentage of the aquifer: arsenic, boron, fluoride, gross alpha activity, molybdenum, uranium, and vanadium. Perchlorate, as a constituent of special interest, was evaluated separately from other inorganic constituents, and had high relative-concentrations in 11.1 percent, moderate in 53.3 percent, and low or not detected in 35.6 percent of the primary aquifers. In contrast to the inorganic constituents, relative-concentrations of organic constituents (one or more) were high in 6.7 percent, moderate in 11.1 percent, and low or not detected in 82.2 percent of the primary aquifers. Of the 237 organic and special-interest constituents analyzed for, 39 constituents were detected (21 VOCs, 13 pesticides, 3 pharmaceuticals, and 2 constituents of special interest). All of the detected VOCs had health-based benchmarks, and five of these—1,1-dichloroethene, 1,2-dibromo-3-chloropropane (DBCP), tetrachloroethene (PCE), carbon tetrachloride, and trichloroethene (TCE)—were detected in at least one sample at a concentration above a benchmark (high relative-concentration). Seven of the 13 pesticides had health-based benchmarks, and none were detected above these benchmarks (no high relative-concentrations). Pharmaceuticals do not have health-based benchmarks. Thirteen organic constituents were frequently detected (detected in at least 10 percent of samples without regard to relative-concentrations): bromodichloromethane, chloroform, cis-1,2-dichloroethene, 1,1-dichloroethene, dichlorodifluoromethane (CFC-12), methyl tert-butyl ether (MTBE), PCE, TCE, trichlorofluoromethane (CFC-11), atrazine, bromacil, diuron, and simazine.