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Paper, a readily available renewable resource, comprises of interwoven cellulosic fibers, which can be functionalized to develop interesting low-cost adsorbent material for water purification. In this study, polyethyleneimine (PEI)-functionalized paper was used for the removal of hazardous pollutants such as Au and Ag nanoparticles, Cr(VI) anions, Ni 2+ , Cd 2+ , and Cu 2+ cations from spiked water samples. Compared to untreated paper, the PEI-coated paper showed significant improvement in adsorption capacities toward the pollutants investigated in this study. Kinetics, isotherm models, pH, and desorption studies were carried out to study the adsorption mechanism of pollutants on the adsorbent surface. Adsorption of pollutants was better described by pseudo-second order kinetics and Langmuir isotherm model. Maximum adsorption of anionic pollutants was achieved at pH 5 while that of cations was at pH > 6. Overall, the PEI-functionalized paper showed interesting Langmuir adsorption capacities for heavy metal ions such as Cr(VI) (68 mg/g), Ni 2+ (208 mg/g), Cd 2+ (370 mg/g), and Cu 2+ (435 mg/g) ions at neutral pH. In addition, the modified paper was also used to remove Ag-citrate (79 mg/g), Ag-PVP (46 mg/g), Au-citrate (30 mg/g), Au-PVP (17 mg/g) nanoparticles from water. Desorption of NPs from the adsorbent was done by washing with 2 M HCl or thiourea solution, while heavy metal ions were desorbed using 1 M NaOH or HNO 3 solution. The modified paper retained its extraction efficiencies upon desorption of pollutants. [ABSTRACT FROM AUTHOR]