The U.S. Geological Survey (USGS) National Water-Quality Assessment (NAWQA) and Toxic Substances Hydrology Programs conducted the National Mercury Pilot Study in 1998 to examine relations of mercury (Hg) in water, bed sediment and fish in streams across the United States, including Alaska and Hawaii. Water and bed-sediment samples were analyzed for total Hg (THg), methylmercury (MeHg), and other constituents; fish were analyzed for THg. Similar sampling was conducted at additional streams across the country in 2002 and 2004-05. This report summarizes sample collection and processing protocols, analytical methods, environmental data, and quality-assurance data for stream water, bed sediment, and fish for these national studies. To extend the geographic coverage of the data, this report also includes four regional USGS Hg studies conducted during 1998-2001 and 2004. The environmental data for these national and regional Hg studies are provided in an electronic format.