The treatment of organic wastewater is of great significance. Carbon nanotube (CNT)/graphene‐based nanomaterials have great potential as absorbent materials for organic wastewater treatment owing to their high specific surface area, mesoporous structure, tunable surface properties, and high chemical stability; these attributes allow them to endure harsh wastewater conditions, such as acidic, basic, and salty conditions at high concentrations or at high temperatures. Although a substantial amount of work has been reported on the performance of CNT/graphene‐based nanomaterials in organic wastewater systems, engineering challenges still exist for their practical application. Herein, the adsorption mechanism of CNT‐ and graphene‐based nanomaterials is summarized, including the adsorption mechanism of CNTs and graphene at the atomic and molecular levels, their hydrophilic and hydrophobic surface properties, and the structure–property relationship required for adsorption to occur. Second, the structural modification and recombination methods of CNT‐ and graphene‐based adsorbents for various organic wastewater systems are introduced. Third, the engineering challenges, including the molding of macroscopically stable adsorbents, adsorption isotherm models and adsorption kinetic behaviors, and reversible adsorption performance compared to that of activated carbon (AC) are discussed. Finally, cost issues are discussed in light of scalable and practical application of these materials.