Decades of acidic deposition have adversely affected aquatic and terrestrial ecosystems in acid-sensitive watersheds in parts of the eastern United States. The national Acid Rain Program (Title IV of the 1990 Clean Air Act Amendments - CAAA) helped reduce emissions of sulfur dioxide (SO₂) and nitrogen oxides (NO_x) and resulted in sharp decreases in the acidity of atmospheric deposition. The decrease in acidic deposition produced a steady decline in the acidity of streams in many poorly buffered waters across the western Adirondacks and parts of the Catskill Mountains of New York. Until recently, however, there has been little evidence of biological recovery in most acid-sensitive streams in both regions. Long-term deposition and stream-chemistry records and fish-community data from quantitative surveys done during 1991–93 and again during 2012–19 at 13 sites in the upper Neversink River and its tributaries were evaluated to determine if chemical and biological recovery were evident in this Catskill Mountain watershed and if they could be linked to regional declines in acidic deposition. Between 1991 and 2019, large decreases in sulfate and nitrate deposition in the basin mirrored declines in total nationwide SO₂ and NO_x emissions. There were corresponding decreases in sulfate and nitrate concentrations in deposition at a National Trends Network station at Frost Valley (NY68) and coincident declines in sulfate concentrations at four long-term monitoring sites in the Neversink River watershed. Mean acid neutralizing capacity and pH increased and inorganic aluminum (Al_i) concentrations from routine summertime samples decreased significantly at most moderately to severely acidified sites between the two study periods. Richness, density, and biomass of fish communities increased at most sites, while the density and biomass of brook trout Salvelinus fontinalis populations increased at fewer sites that were undergoing chemical recovery. Although recovery is far from complete, trends in deposition chemistry, water quality, and fish assemblages in streams of the upper Neversink watershed indicate that the 1990 CAAA is having positive impacts on aquatic ecosystems in the Catskill Mountain region, New York.