Graphene-based adsorbents show great potential for application in the field of environmental pollution treatment due to their unique two-dimensional structure, high specific surface area, and tunable surface chemistry. This paper reviews the research on the application of graphene and its derivatives as novel adsorbents in the field of wastewater treatment in recent years, focusing on the preparation and functionalization of graphene-based adsorbents, as well as their adsorption performance and mechanism of action in the removal of inorganic and organic pollutants, and provides an outlook on the future directions of the research on graphene-based adsorbents. The analysis in this paper focuses on the functionalization of graphene-based adsorbents by introducing magnetic particles, hybridization with other materials, and grafting with polymers. The modified graphene-based adsorbents showed significant adsorption and removal of pollutants and were easy to recycle and regenerate. The adsorption of pollutants on graphene-based adsorbents is mainly carried out through π–π interaction, hydrogen bonding, and electrostatic interaction, which is related to the structure of the pollutants. Future research directions on graphene-based adsorbents should focus on in-depth adsorption mechanism studies and the development of cost-effective graphene-based adsorbents for wastewater treatment.