An evaluation of water-quality data from streams that receive stormwater runoff from a segment of Interstate Highway 85 in North Carolina indicated increased levels of many constituents compared to levels in nearby undeveloped basins. Additional data collected from a network of dry and wet atmospheric deposition collectors, lysimeter samples, soil surveys, wind measurements, and road sweepings helped define the general sources and migration of chemical substances near the highway. The eight study basins, located in a rural area in the Piedmont of North Carolina, had a combined area of 17.5 square miles and drained a 4.8-mile-long segment of the interstate. The average traffic flow along this section was 25,000 vehicles per day. During storm runoff, streamflow in basins traversed by the highway rose and fell more rapidly than that in the undeveloped basins. This more rapid response is due to the impervious, paved area of the basins and the manmade drainage systems designed to rapidly move water off the highway. Alkalinity, specific conductance, and concentrations of calcium, sodium, and chloride were greater at the highway stations than in the undeveloped basins as a result of highway salting for control of ice. Specific conductance and concentrations of dissolved and total nitrogen peaked at the beginning of each storm event. The data indicated that, for the study basins, highway runoff had little or no effect on suspended sediment, water temperature, dissolved oxygen, and pH. However, the pH at all stations decreased during stormflow because the rainfall drained off by the streams had pH values less than 5.7. High metals concentrations were found in the soils within 100 feet of the highway and in the soil water infiltrating the soil zone. Chromium, copper, nickel, and zinc concentrations in the streams near the highway generally were above the maximum levels recommended by the U.S. Environmental Protection Agency (EPA) for the protection of aquatic life. Lead and cadmium concentrations frequently exceeded the maximum levels recommended by the EPA for drinking water. The highway is a source of contaminants to surrounding areas. Particulate and metal loads in dustfall and chemical-constituent concentrations in soils decrease exponentially with distance from the highway. The highest concentrations of contaminants were found on the downwind side. Increased concentrations of metals (cadmium, chromium, iron, lead, nickel, and zinc) in rainfall were observed in samples collected near the highway and in samples collected approximately one-half mile away. Material loading due to dustfall was greater than loading due to rainfall. Loading due to saltated particles, those heavier particles bounced along the highway surface, was higher than loading due to dustfall. Saltation loads were greatest during the winter months because of highway deicing and sanding, which supplied an estimated two-thirds of the saltated materials. The remaining one-third of the saltated load came primarily from the deposition of particles from vehicles. Some of the greatest constituent concentrations were measured in the soil water sampled from the lysimeters located adjacent to the highway.