{Benthic diatoms and water chemistry were sampled from 49 stream sites in the Mid-Atlantic Highlands region of the US to evaluate the use of diatoms as indicators of environmental conditions in streams across varying geographic and ecoregional areas. Diatom samples were collected from depositional and erosional habitats in a randomly selected reach in each stream site. Patterns of diatom species distributions in relation to environmental variables were determined using canonical correspondence analysis. Diatom species in both habitats were highly correlated with a pH gradient. A second gradient was correlated with variables that were commonly associated with agricultural runoff such as turbidity and total phosphorus. The relationship between diatoms and major environmental variables was quantified with regression and calibration models. The correlation between diatom-inferred and observed pH was high (r2 = 0.90). Cross-validation with jackknifing showed that pH models were reasonably robust (r2 = 0.69 for depositional habitats