This review article focuses on the surface adsorptive properties of carbon nanotubes and their use in the removal of organic environmental contaminants from water. An introduction to the prevalent organic contaminants as well as some emerging contaminants such as pharmaceuticals and personal care products in aquatic environment are briefly discussed. The growth and surface modification techniques of carbon nanotubes and their implication on the adsorption potential of CNTs are examined. Adsorption capacity and affinity of organic contaminants on carbon nanotubes and parameters affecting such adsorption process including the environmental chemistry such as competition from co-existing environmental contaminants are summarized. The recent use of molecular dynamics simulation to investigate the molecular mechanism and adsorption phenomenon near carbon nanotube surfaces are briefly reviewed. Some of our recent MD simulation investigations of adsorption mechanisms and interactions between organic contaminants and CNT surfaces are presented. New developments and potential directions on adsorption-based CNT applications in water purification are discussed.