PFAS, per- and polyfluorinated alkyl substances, are man-made chemicals used in goods such as nonstick cookware, fabric coating, makeup, and lithium batteries. Their extreme thermal and chemical stability, due to strong C–F bonds, makes them ideal for commercial use but also environmentally persistent. These compounds have been increasingly linked to cancer, hormonal problems, and birth defects, and are now often detected in drinking water. Short-chain PFAS, defined as having fewer than 7 carbons on their carbon-fluorine backbone, are more mobile, difficult to degrade, and likely to enter human systems. Therefore, it is important to develop degradation methods to fully eliminate these PFAS. We report an electrochemical process to degrade short-chain PFAS. Using 19-F NMR, ion chromatography, and ion selective electrode, we were able to observe up to 100% degradation and defluorination of PFBA. Our process showed effectiveness against other short-chain PFAS, including trifluoroacetic acid (TFA), hexafluoropropylene oxide dimer acid (HFPO-DA, also known as Gen-X), and 4:2 fluorotelomer sulfonate (4:2 FTS). This electrochemical system enables scalable degradation of short-chain PFAS.