As the world human population and industrialization keep growing, the water availability issue has forced scientists, engineers, and legislators of water supply industries to better manage water resources. Pollutant removals from wastewaters are crucial to ensure qualities of available water resources (including natural water bodies or reclaimed waters). Diverse techniques have been developed to deal with water quality concerns. Carbon based nanomaterials, especially carbon nanotubes (CNTs) with their high specific surface area and associated adsorption sites, have drawn a special focus in environmental applications, especially water and wastewater treatment. This critical review summarizes recent developments and adsorption behaviors of CNTs used to remove organics or heavy metal ions from contaminated waters via adsorption and inactivation of biological species associated with CNTs. Foci include CNTs synthesis, purification, and surface modifications or functionalization, followed by their characterization methods and the effect of water chemistry on adsorption capacities and removal mechanisms. Functionalized CNTs have been proven to be promising nanomaterials for the decontamination of waters due to their high adsorption capacity. However, most of the functional CNT applications are limited to lab-scale experiments only. Feasibility of their large-scale/industrial applications with cost-effective ways of synthesis and assessments of their toxicity with better simulating adsorption mechanisms still need to be studied.