In recent years, graphene-based materials (GBMs) have been regarded as the core technology in diverse research fields. Consequently, the demand for large-scale synthesis of GBMs has been increasing continuously for various fields of industry. These materials have become a competitive adsorbent for the removal of environmental pollutants with improved adsorption capacity and cost effectiveness through hybridization or fabrication of various functionalities on their large surface. In particular, their applicability opens up new avenues for the adsorptive removal of volatile organic compounds (VOCs) (e.g., through the build-up of efficient air purification systems). This review explored the basic knowledge and synthesis approaches for GBMs and their performances as adsorbent for VOC removal. Moreover, the mechanisms associated with the VOC removal were explained in detail. The performance of GBMs has also been evaluated along with their present limitations and future perspectives.