Per- and polyfluoroalkyl substances (PFAS) are man-made organofluorine chemicals that can contaminate environmental waters and have gained worldwide attention over the past two decades. PFAS are most frequently detected by mass spectrometric targeted analysis methods which may not detect all the PFAS in samples. This report describes the investigation of adsorbable organofluorine (AOF) with detection by combustion ion chromatography (CIC) for detection of PFAS in surface waters and wastewaters that adsorb to granular activated carbon (GAC) with the recognition that this technique measures more than just PFAS. Overall mean recoveries of 77–120% were obtained in 17 of the 18 tested surface water and wastewater matrices spiked with perfluoropentane sulfonate (PFPeS) and 55–119% mean recoveries were obtained in 11 of the 12 surface water and wastewater matrices spiked with a PFAS mixture. Poor method performance (34–39% mean recoveries) was observed in landfill leachate wastewater. Method detection limits of 1.4–2.2 μg L⁻¹ were achieved using 100 mL sample volumes adsorbed onto commercially available GAC. This report demonstrates that this AOF technique can be a useful screening tool for estimating organofluorine concentrations when PFAS contamination is suspected.