• GO-PDMAEMA nanocomposites synthesized via ATRP show high Cr(VI) adsorption capacity up to 164.4 mg·g−1.
• Adsorption follows pseudo-second-order kinetics and is controlled by both surface adsorption and intraparticle diffusion.
• The adsorbents retain over 85% capacity after five adsorption-desorption cycles, indicating good reusability.
• Electrostatic interactions between protonated nitrogen groups and Cr(VI) anions drive the efficient removal.
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