Data on the chemical composition of soil-water samples were collected quarterly from three watersheds in Shenandoah National Park, Virginia, from September 1999 through July 2000. The soil-water samples were analyzed for specific conductance and concentrations of sodium, potassium, calcium, magnesium, ammonium, chloride, nitrate, sulfate, acid-neutralizing capacity, silica, and total monomeric aluminum. The soil-water data presented in this report can be used to support water-quality modeling of the response of streams to episodic acidification. Laboratory analytical data as well as laboratory quality-assurance information also are presented.