Demand for clean and safe drinking water is a global challenge because of water scarcity, growth of human population, urbanization, and anthropogenic pollution. Purification of water involves removal of small molecules and ions from ground water addressed as “emerging contaminants” which are extremely mobile and toxic in nature, do not degrade or hydrolyze easily, and highly soluble in water resulting in bioaccumulation. Most of the current water treatment systems have complex deficiencies that affect their overall performance. We have synthesized carbon nanostructures assisted ion exchange resins in aqueous medium that help remove these emerging contaminants in a fast, easy, and high capacity manner while supporting less contact time and low transmembrane resistance primarily achieved using thin film assemblies. We have developed a novel sonochemistry assisted atom transfer radical polymerization (SONO-ATRP) process for synthesis of polyelectrolyte anion exchange resins in water without use of any external initiator or reducing agents while using only a few ppm of catalyst. We successfully performed high-density functionalization of polyelectrolyte anion exchange resin strands onto single walled carbon nanotubes sidewalls using the SONO-ATRP process while at low reaction temperatures thereby providing a less energy intensive alternative for green chemistry. We have developed green processes to defluorinate fluorographite in water and simultaneously perform covalent grafting of anionic short brushes of poly(vinyl benzyl trimethylammonium chloride) to its surface under mild reaction conditions without need of any external reactive reagents. Field Emission Scanning Electron microscopy of thin film of functionalized carbon nanotubes demonstrated pin-hole free mesoporous architecture illustrating scaffold robustness while thin films of functionalized fluorographite exhibited stacked arrangement of plate-like structures. Exfoliation and functionalization of fluorographite was revealed through Transmission Electron Microscopy. Both the resins demonstrated high water flux (>1500 L m^(-2) h^(-1) bar^(-1)) due to their intrinsic architecture and high percent removal (>90%) of contaminants due to the tortuous path length during molecular transport through the membrane. These properties enable adsorption of impurities at environmentally relevant concentrations. These materials exhibited facile regeneration and reusage of the thin films, thus supporting sustainability. In conclusion, these processes abide by the principles of green chemistry and their processability opens new avenues for smart point-of-use water purification systems.