Excess nitrogen (N) in terrestrial ecosystems can arise from anthropogenically-increased atmospheric N deposition, a phenomenon common in eastern US forests. In spite of decreased N emissions over recent years, atmospheric concentrations of reactive N remain high in areas within this region. Excess N in forests has been shown to alter biogeochemical cycling of essential plant nutrients primarily via enhanced production and leaching of nitrate, which leads to loss of base cations from the soil. The purpose of our study was to investigate this phenomenon using a multifaceted approach to examine foliar nutrients of two herbaceous layer species in one N-treated watershed (WS3—receiving aerial applications of 35 kg N/ha/yr as ammonium sulfate, from 1989 to the present) and two untreated reference watersheds at the Fernow Experimental Forest, WV, USA. In 1993, we analyzed foliar tissue of Viola rotundifolia, a dominant herb layer species and prominent on all seven sample plots in each watershed. In 2013 and 2014, we used foliar tissue from Rubus allegheniensis, which had become the predominant species on WS3 and had increased, though to a lesser extent, in cover on both reference watersheds. Foliar N and potassium (K) were higher and foliar calcium (Ca) was lower on WS3 than on the reference watersheds for both species. Magnesium (Mg) was lower on WS3 for Viola, but was not different among watersheds for Rubus. Results support the stream chemistry-based observation that excess N lowers plant-available Ca and, to a lesser degree, Mg, but not of K. Foliar manganese (Mn) of Rubus averaged >4 times that of Viola, and was >50% higher on WS3 than on the reference watersheds. A Mn-based mechanism is proposed for the N-meditated increase in Rubus on WS3. Data suggest that excess N deposition not only alters herb community composition and biogeochemical cycling of forest ecosystems, but can do so simultaneously and interactively.