Nanocomposites containing graphene oxide (GO), polyethyleneimine (PEI), and chitosan (CS) were synthesized for chromium(VI) and copper(II) removal from water. Response surface methodology (RSM) was used for the optimization of the synthesis of the CS-PEI-GO beads to achieve simultaneous maximum Cr(VI) and Cu(II) removals. The RSM experimental design involved investigating different concentrations of PEI (1.0-2.0%), GO (500-1500 ppm), and glutaraldehyde (GLA) (0.5-2.5%), simultaneously. Batch adsorption experiments were performed to obtain responses in terms of percent The optimum bead composition contained 2.0% PEI, 1500 ppm GO, and 2.08% GLA, and allowed Cr (VI) and Cu(II) removals of up to 91.10% and 78.18%, respectively. Finally, characterization of the structure and surface properties of the optimized CS-PEI-GO beads was carried out using X-ray diffraction (XRD), porosity and BET surface area analysis, scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), which showed favorable adsorbent characteristics as given by a mesoporous structure with high surface area (358 m 2 g À1 ) and plenty of surface functional groups. Overall, the synthesized CS-PEI-GO beads were proven to be effective in removing both cationic and anionic heavy metal pollutants.