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As concerns rise about the health risks posed by per- and polyfluoroalkyl substances (PFAS) in the environment, there is a need to understand how these pollutants accumulate at environmental interfaces. Untangling the details of molecular adsorption, particularly when there are potential interactions with other molecules in environmental systems, can obscure the ability to focus on a particular contaminant with molecular specificity. Often adsorption studies of environmental interfaces require a reductionist approach, where laboratory experiments may not be fully tractable to environmental systems. In this work, we study polyfluorinated dodecylphosphonic acid (F21-DDPA) at the aqueous surfaces of distilled water (the most reduced “environmental” surface) and river water to explore the use of vibrational sum-frequency (VSF) spectroscopy as an experimental probe of fluorinated contaminants at natural environmental surfaces. We demonstrate how VSF spectroscopy offers advantages over nonspecific surface tension measurements when measuring PFAS adsorption isotherms at river water surfaces. VSF spectra of the C–F stretching region selectively probe the presence of F21-DDPA and can be used to extract meaningful structural insights and calculate surface concentrations, even at the complex river water surface. This study highlights the potential for VSF spectroscopy to be developed as a probe of fluorinated contaminants at natural environmental interfaces.