We conducted field studies to determine the levels of acid and aluminum (Al) that affect survival, smolt development, ion homeostasis, and stress in Atlantic salmon (Salmo salar) smolts in restoration streams of the Connecticut River in southern Vermont, USA. Fish were held in cages in five streams encompassing a wide range of acid and Al levels for two 6-day intervals during the peak of smolt development in late April and early May. Physiological parameters were unchanged from initial sampling at the hatchery and the high water quality reference site (pH > 7.0, inorganic Al < 12 μg·L^-1). Mortality, substantial loss of plasma chloride, and gill Na⁺/K⁺-ATPase activity, and elevated gill Al occurred at sites with the lowest pH (5.4-5.6) and highest inorganic Al (50-80 μg·L^-1). Moderate loss of plasma chloride, increased plasma cortisol and glucose, and moderately elevated gill Al occurred at less severely impacted sites. Gill Al was a better predictor of integrated physiological impacts than water chemistry alone. The results indicate that Al and low pH under field conditions in some New England streams can cause mortality and impair smolt development in juvenile Atlantic salmon and provide direct evidence that episodic acidification is impacting conservation and recovery of Atlantic salmon in the northeastern USA.