Long-term monitoring of water quality responses to natural and anthropogenic perturbation of watersheds informs policies for managing natural resources. Dissolved organic carbon (DOC) and nitrate (NO₃⁻) in streams draining forested landscapes provide valuable information on ecosystem function due to their biogeochemical reactivity and solubility in water. Here we evaluate a 20-year record (2001−2021) of biweekly stream-water samples (n > 3000) and continuous discharge in three forested catchments in the Adirondack region of New York to investigate and interpret long-term trends in DOC and NO₃⁻ concentrations. Results from the intensively monitored catchments were compared with data from synoptic surveys of streams throughout the Adirondack region. A weighted regressions on time, discharge, and season (WRTDS) model, used to estimate daily flow-normalized concentrations, determined that DOC increased by ~30 to 50 % while NO₃⁻ decreased by ~50 to 70 % over the study period. The large amount of data from catchments with different soil properties permitted us to assess the relative effects of hydrology, season, and land cover factors on temporal trends in DOC and NO₃⁻ concentrations. We found weak evidence of climatic forcing of long-term increases in DOC, and instead contend that declining ionic strength in precipitation linked to declining anthropogenic acid deposition is driving DOC trends in stream waters. Nitrate concentrations were more variable but clearly decreased in recent years possibly related to declining N deposition. The recent increase in DOC:NO₃⁻ in all catchments indicates a major shift in stream stoichiometry that reflects changes in ecosystem functioning that may have important biogeochemical implications for terrestrial as well as aquatic ecosystems.