In spite of overall improvements in air and water quality, biological stress from low pH and high concentrations of inorganic aluminum continue to impact fish and fish habitat in northeastern North America, with independent and interactive effects on individuals, populations and communities. Integrative indicators can therefore be useful in monitoring both impact and recovery across multiple scales. Using coupled water chemistry (pH, conductivity, and base cation and inorganic aluminum concentration), geographic (site elevation and watershed area) and biological (fish diversity, fish abundance, gill aluminum concentration and gill physiology) data, we developed an integrated indicator of acid aluminum stress across the White and Green mountains in central New England, USA. As has been established in a number of previous studies, preliminary analysis clearly indicated that across all sites, inorganic aluminum concentration was consistently greatest during the spring season. Structural Equation modelling (SEM) revealed that toxic conditions (concurrent low pH and high concentrations of inorganic aluminum) were well summarized with an integrated toxicity score, related to both base cation concentrations and elevation, with sites at higher elevations more likely to experience toxic conditions as well as low base cation concentrations. As hypothesized, fish diversity and abundance were negatively related to toxicity score. In spite of considerable variation among individuals, gill aluminum was positively related to toxicity score for both Atlantic salmon and brook trout. Observed elevated gill aluminum levels associated with reduced gill metabolic activity in Atlantic salmon smolts from impacted systems likely result in impaired osmoregulatory function and seawater tolerance. Overall, our results suggest that the integrated toxicity score metric is strongly associated with a syndrome of physiological stress, reduced abundance, and low species diversity for stream fishes in New England and can likely serve as a reliable indicator of continued impairment or recovery of acid-aluminum vulnerable systems in this ecoregion.