© 2021 Elsevier B.V.In this study, the synthesis of a novel arginine-functionalized polyaniline/FeOOH (Arg-PANI@FeOOH) composite for hazardous Hexavalent chromium ions (Cr(VI)) removal from wastewater was reported. The SEM, EDS, FTIR, XRD, and PZC measurements were used to characterize the as-developed Arg-PANI@FeOOH composite. Batch adsorption experiments were used to investigate the influence of pH, temperature, contact time, Arg-PANI@FeOOH amount, initial Cr(VI) concentration and coexisting ions on the efficiency of Cr(VI) removal. The Cr(VI) adsorption was much more advantageous at lower pH values, reflecting that the electrostatic interactions were the main driving forces that govern Cr(VI) binding mechanism on the Arg-PANI@FeOOH surface. The experimental data showed good fitness to the pseudo-second-order kinetics and Langmuir isotherm. The Cr(VI) species highest monolayer coverage capacity onto Arg-PANI@FeOOH was 682.30 mg g−1. The adsorption of Cr(VI) onto the Arg-PANI@FeOOH is spontaneous via an endothermic reaction. The competing anions were not affected the Cr(VI) adsorption, demonstrating that the Arg-PANI@FeOOH selectively adsorb Cr(VI) ions. The developed Arg-PANI@FeOOH material demonstrated good reusability up to five regeneration cycles. The process capability to predict the practical aptitude of Arg-PANI@FeOOH adsorbent to remove Cr(VI) from aqueous solutions was successfully applied. As a result, the adsorption of Cr(VI) onto Arg-PANI@FeOOH composite is a capable process for full-scale wastewater purification purposes. This paper provides relevant findings for a polyaniline-based adsorbent for the efficient removal of Cr(VI) from wastewater.