Colorimetric Cl- data from natural solutions that contain dissolved organic carbon (DOC) may be biased high. We evaluated aquatic Cl- concentrations in ecosystem compartments at the Bear Brook Watershed, Maine, and from lakes in Maine, using ion chromatography and colorimetry. DOC imparts a positive interference on colorimetric Cl- results proportional to DOC concentrations at approximately 0.8 ??eq Cl-/L per mg DOC/L. The interference is not a function of Cl- concentration. The resulting bias in concentrations of Cl- may be 50% or more of typical environmental values for Cl- in areas remote from atmospheric deposition of marine aerosols. Such biased data in the literature appear to have led to spurious conclusions about recycling of Cl- by forests, the usefulness of Cl- as a conservative tracer in watershed studies, and calculations of elemental budgets, ion balance, charge density of DOC, and dry deposition factors.