Geothermal waters in Yellowstone National Park contribute large quantities of arsenic to the headwaters of the Madison River. Water in some Quaternary and Tertiary valley-fill deposits along the Madison and upper Missouri Rivers also is locally enriched in arsenic. Arsenic in surface and ground water in these valleys is an important public- health concern because arsenic concentrations frequently exceed the State of Montana water- quality human health standard of 18 micrograms per liter as well as the U.S. Environmental Protection Agency Maximum Contaminant Level of 50 micrograms per liter. This report presents hydrologic and water-quality data for the Madison and upper Missouri Rivers and selected tributaries, irrigation supply canals or ditches, drains, springs and seeps, for Lake Helena, and for ground water in adjacent areas. Hydrologic and water-quality data were collected and compiled to provide information to more fully understand the extent, magnitude, and source of arsenic in surface and ground water along the Madison and upper Missouri Rivers; to assess, to the extent possible, the mechanisms that control arsenic concentrations; and to assess the effect of irrigation on arsenic concentrations. Hydrologic and arsenic- concentration data were collected by the U.S. Geological Survey and other agencies for 104 surface-water sites and 273 ground-water sites during this and previous studies. The quality of analytical results for arsenic concentrations was evaluated by quality-control samples that were submitted from the field and analyzed in the laboratory with routing samples. Quality-control samples consisted of replicates, standard reference samples, interlaboratory comparison samples, and field blanks.