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Graphene-based nanomaterials have attracted researchers from various fields due to their extraordinary physical, chemical, and electrochemical properties. An emerging class of graphene-based nanostructures and nanocomposites is considered to be a promising solution to various types of environmental pollution. The electro-Fenton process is one of the easy and effective approaches to treating a wide range of organic pollutants in a liquid medium. The usage of graphene-based electrodes in the electro-Fenton process is considered to be a promising and cleaner way to produce reactive oxygen species to mineralize organic contaminants rapidly. Graphene derivatives are used to immobilize various heterogeneous Fenton catalysts for improved catalytic activity, stability, and reusability. In this review, the importance of graphene-based materials in improving the performance efficiency in the electro-Fenton process is presented along with an enhancement mechanism through the following discussions: (i) the significance of oxygen functional groups and nitrogen doping on graphene layers to enhance the two-electron oxygen reduction reactions; (ii) the advantages of iron-loaded graphene-based materials as catalysts and composite electrodes for the enhanced production of reactive oxygen species; (iii) a summary of various forms of graphene-based materials, modifications in their chemical structure, properties, and applications in the electro-Fenton process to remove organic contaminants.