Anthropogenic and industrial emissions have resulted in historically high levels of acidic deposition into central Appalachian forests. Despite the reduction in acidic inputs due to legislation curbing industrial emissions in the United States, continued N deposition may impact forest ecosystems. Soil and foliar samples were collected from four high elevation red spruce sites along a modeled gradient of historic N deposition. The three most abundant tree species at all sites, Acer rubrum L., Betula alleghaniensis Britt., and Picea rubens Sarg., were sampled. Bulk soil beneath the canopies of individual trees were collected from the top 15-cm and separated into organic and mineral fractions for analysis. Mehlich-III soil extracts of soil fractions and foliar digests from these trees were subjected to elemental analysis. Soil N concentrations supported the presence of a N deposition gradient: in organic horizon soil fractions, N concentrations were driven by precipitation volume and elevation; whereas in mineral soil fractions, N concentration was explained by modeled N deposition rate and elevation. In organic fractions, significant reductions in Ca, K, and P were evident as N deposition increased, whereas the Ca:Sr ratio increased. Foliar Ca, K, and Sr declined in foliage with increasing N deposition, with concomitant increases in foliar Ca:Sr ratios. Although the three species were sympatric in mixed stands at all four sites, the foliar-soil nutrient associations differed among them across the gradient, indicating differential uptake and cycling of nutrients/metals by these forest tree species.