Although diamond electrodes are widely used in the field of electroanalysis and sensing, their application in the field of environmental engineering has yet to be fully realized. Many research studies have considered their potential application in water and wastewater treatment, where the in-situ electrochemical process can avoid the need for chemical additives by facilitating the oxidation of pollutants on the electrode surface or mediated by electrochemically synthesized oxidants in solution. Diamond-based electro-oxidation can effectively treat a number of organic micropollutants and is now being evaluated for the abatement of perfluoroalkyl and polyfluoroalkyl substances, which pose health concerns and are ubiquitous recalcitrant environmental contaminants. To move implementation of diamond-based electro-oxidation forward, the integration of modifications and codopants to yield more advanced electrode materials needs to be further developed and understood. The progress and current strategies associated with diamond electrode modifications for perfluoroalkyl and polyfluoroalkyl substances abatement as well as future considerations are discussed.