High-elevation aquatic ecosystems in Mount Rainier and North Cascades National Parks are highly sensitive to atmospheric deposition of nitrogen and sulfur. Thin, rocky soils promote fast hydrologic flushing rates during snowmelt and rain events, limiting the ability of basins to neutralize acidity and assimilate nitrogen deposited from the atmosphere. Potential effects of nitrogen and sulfur deposition include episodic or chronic acidification of terrestrial and aquatic ecosystems. In addition, nitrogen deposition can cause eutrophication of water bodies and changes in species composition in lakes and streams. This report documents results of a study performed by the U.S. Geological Survey, in cooperation with the National Park Service, of the effects of atmospheric deposition of nitrogen and sulfur on surface-water chemistry in Mount Rainier and North Cascades National Parks. Inorganic nitrogen in wet deposition was highest in the vicinity of North Cascades National Park, perhaps due to emissions from human sources and activities in the Puget Sound area. Sulfur in wet deposition was highest near the Pacific coast, reflecting the influence of marine aerosols. Dry deposition generally accounted for less than 30 percent of wet plus dry inorganic nitrogen and sulfur deposition, but occult deposition (primarily fog) represents a potentially substantial unmeasured component of total deposition. Trend analyses indicate inorganic nitrogen in wet deposition was relatively stable during 1986-2005, but sulfur in wet deposition declined substantially during that time, particularly after 2001, when emissions controls were added to a large powerplant in western Washington. Surface-water sulfate concentrations at the study site nearest the powerplant showed a statistically significant decrease between 2000 and 2005-06, but there was no statistically significant change in alkalinity, indicating a delayed response in surface-water alkalinity. Seasonal patterns in surface-water chemistry and streamflow are strongly influenced by melting of seasonal snowpacks, which release large amounts of dilute, slightly acidic water to terrestrial and aquatic ecosystems during spring snowmelt. Concentrations of sulfate, alkalinity, and base cations in surface water declined rapidly during snowmelt, then gradually recovered during summer and fall. Preferential elution of acidic solutes from the snowpack at the beginning of snowmelt may cause episodic acidification in small alpine streams; evidence is provided by a stream sample collected at one of the sites during spring 2006 that was acidic (pH = 4.8, alkalinity = -18 microequivalents per liter) and had high concentrations of nitrate and sulfate and low concentrations of weathering products. Rain-on-snow events caused sharp declines in specific conductance, which was measured continuously using an in-stream sensor. A strong correlation was observed between measured specific conductance and measured alkalinity (r2 = 0.76), permitting estimation of alkalinity from specific-conductance data using a regression equation. Estimated alkalinity declined by an order of magnitude during the rain-on-snow events, in one case to 8 microequivalents per liter. Actual declines in alkalinity might be greater because the regression equation accounts only for dilution effects; at low concentrations, the relation between specific conductance and alkalinity is likely to be nonlinear and have a negative intercept (negative alkalinity). Thus, episodic acidification is possible during rain-on-snow events. The scale of episodic acidification is unknown, but if it occurs, it could have detrimental effects on aquatic life and amphibians. Historical lake-survey data indicate that most lakes are oligotrophic and have low nitrogen and phosphorus concentrations. Nitrogen limitation is more common in lakes in Mount Rainier National Park than in North Cascades National Park due to higher nitrate concentrations at North Cascades. T