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The Athabasca oil sands region (AOSR) in north-eastern Alberta, Canada, contains the world's third largest known bitumen deposit. Oil sands (OS) operations produce emissions known to contribute to acidic and alkaline deposition, which can alter the chemistry of the receiving surface waters, including dissolved organic carbon (DOC). Little is known regarding the natural variability of aquatic DOC among lakes within the AOSR. Surface-water data from 50 lakes were analyzed; variables known to be associated with the light-absorptive properties of DOC (true color [TC]) were evaluated to investigate the potential variability of chromophoric DOC (CDOC). Comparison of TC and DOC revealed two distinct "high" (H) and "low" (L) lake subpopulations, the former being characterized by high relative TC and low DOC, and the latter by the inverse. The H lakes were defined by variables known to be associated with CDOC, while L lakes appeared well-buffered potentially owing to groundwater inputs. The divergent optical properties between subpopulations appeared partially attributable to pH-limited Fe complexation. Trajectory analysis indicated that H lakes most likely to receive atmospheric deposition from OS sources experienced significantly lower pH. These results are contrary to previous studies that found OS emissions to have minimal acidifying effect over lakes throughout the AOSR.