The quantity and composition of dissolved organic carbon (DOC) exported from upland soils to surface waters is a key link in the global carbon cycle and economically important for treating potable waters. The relationship between ultraviolet (UV) absorbance and DOC concentrations can be used to infer changes in the proportion of hydrophobic (aromatic, recalcitrant) carbon and hence biodegradability of DOC. This study describes a significant change in the relationship between UV absorbance and DOC over 22 years at two upland moorland catchments in Scotland, UK. Despite increases in long-term DOC concentrations, analysis suggests that the proportion of hydrophobic material has declined. A statistical mixed-effect modeling approach was used to examine the likely mechanisms that could explain these observations. Annual nonmarine sulfate load was the only significant forcing factor that could explain the observed long-term trend in the UV absorbance-DOC relationship at both sites. It is hypothesized that enhanced heterotrophic decomposition of organic matter and increased solubility of carbon compounds in soils where sulfate driven acidification is being reversed are the dominant mechanisms behind this change in DOC composition. These trends will impact on carbon substrate dynamics by potentially increasing biodegradability of exported organic matter, influencing carbon cycling in terrestrial and aquatic ecosystems.