Water security is a top concern for social well-being and dramatic changes in the availability of freshwater have occurred as a result of human uses and landscape management. Elevated nutrient loading and perturbations to major ion composition have resulted from human activities and have degraded freshwater resources. This study addresses the emerging nature of stream water quality in the 21st century through analysis of concentrations and trends in a wide variety of constituents in streams and rivers of the U.S. Concentrations of fifteen separate water quality parameters including nutrients, major ions, sediment, and specific conductance were analyzed over the period 1982-2012 and a targeted trend analysis was performed from 1992-2012. Although environmental policy is geared toward addressing the long-standing problem of nutrient overenrichment, these efforts have had uneven success, with decreasing nutrient concentrations at urbanized sites and little to no change at agricultural sites. However, freshwaters are being salinized rapidly in all human-dominated land use types. Increasing salinity negatively affects biodiversity, mobilizes sediment-bound contaminants, and increases lead contamination of drinking water but the effects are poorly quantified. Therefore, while efforts to control nutrients are ongoing, rapid salinity increases are ushering in a new set of poorly-defined issues.