Olives are inedible because of high levels of bitter phenolics (e.g., oleuropein) which are removed during commercial olive processing. Current commercial processing methods are highly water-intensive, produce toxic wastewater, and are environmentally unsustainable. To address this, macroreticular polymeric resins were used to assist debittering and decrease water use. Amberlite resins XAD4, XAD16N, XAD7HP, and FPX66 were evaluated for the ability to adsorb bitter and/or high-value phenolic compounds (i.e., oleuropein, ligstroside, oleuropein aglycone, ligstroside aglycone, oleocanthal, oleacein, and hydroxytyrosol) from whole olives during typical brine storage. All resins effectively adsorbed oleuropein and ligstroside. FPX66 reduced oleuropein in whole olives suspended in a 1.0% acetic acid brine to 0.635 mg/kg wet weight in 2.5 months with no further processing. This concentration is below levels measured in commercial California-style black ripe olives (0.975 mg/kg wet weight). Resins in storage brines effectively decrease levels of bitter phenolic compounds without additional lye processing. Excellent recoveries of high-value phenolic compounds are obtained from resins (e.g., 80.2 ± 3.3% to 89.4 ± 8.9% hydroxytyrosol).