Under the United States Clean Air Act Amendments of 1977, a class I designation safeguards wilderness areas from the negative effects of new sources of air pollution. We monitored streamwater chemistry in the class I Lye Brook Wilderness in southwestern Vermont from May 1994 through August 1995. Stream samples were collected biweekly at nine sampling locations throughout the wilderness and were analyzed for major cations and anions, dissolved organic carbon, pH, and acid-neutralizing capacity. Eight of nine sites sampled had mean annual acid neutralizing capacity values below zero. During the study period, decreases in streamwater acid neutralizing capacity values were caused primarily by SO(4)(2-). At some sites, however, NO(3) (-) and naturally occurring, weak organic acids were seasonally important. During high discharge, the low pH and high concentrations of inorganic monomeric Al were at levels that are toxic to acid-sensitive aquatic species. Watershed mass balances were calculated to determine annual gains or losses for measured ions. These budgets indicate that S inputs and outputs were nearly equal, there was a net loss of base cations, and a net gain in N. How long these watersheds can continue to assimilate additional N inputs is unknown.