The biogeochemical cycling of sulfur (S) was studied during the 2000 snowmelt at Sleepers River Research Watershed in northeastern Vermont, USA using a hydrochemical and multi-isotope approach. The snowpack and 10 streams of varying size and land use were sampled for analysis of anions, dissolved organic carbon (DOC), ³⁵S activity, and δ³⁴S and δ¹⁸O values of sulfate. At one of the streams, δ¹⁸O values of water also were measured. Apportionment of sulfur derived from atmospheric and mineral sources based on their distinct δ³⁴S values was possible for 7 of the 10 streams. Although mineral S generally dominated, atmospheric-derived S contributions exceeded 50% in several of the streams at peak snowmelt and averaged 41% overall. However, most of this atmospheric sulfur was not from the melting snowpack; the direct contribution of atmospheric sulfate to streamwater sulfate was constrained by ³⁵S mass balance to a maximum of 7%. Rather, the main source of atmospheric sulfur in streamwater was atmospheric sulfate deposited months to years earlier that had microbially cycled through the soil organic sulfur pool. This atmospheric/pedospheric sulfate (pedogenic sulfate formed from atmospheric sulfate) source is revealed by δ¹⁸O values of streamwater sulfate that remained constant and significantly lower than those of atmospheric sulfate throughout the melt period, as well as streamwater ³⁵S ages of hundreds of days. Our results indicate that the response of streamwater sulfate to changes in atmospheric deposition will be mediated by sulfate retention in the soil.