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[Display omitted] • Polyethyleneimine functionalized chitosan aerogel is prepared via a facile pathway. • PCA-3 possesses 3D network structure and reversible compressibility. • PCA-3 has superior adsorption ability to Cr(VI) with maximum capacity of 445.3 mg/g. • PCA-3 can filter 7.4 L of real Cr wastewater with a concentration of 52.88 mg L−1. • PCA-3 can reduce the accumulation of Cr(VI) in wheat roots and leaves. Here we unveiled a novel polyethyleneimine (PEI) functionalized chitosan (CS) aerogel (PCA) with three-dimensional (3D) porous network structure and superior reversible compression property and investigated its adsorption behavior toward Cr(VI). The kinetic study displayed that the adsorption of Cr(VI) ions followed the pseudo-second-order model, indicating the adsorption was such as to depend on the chemical reaction between Cr(VI) ions and PCA. Notably, the maximum adsorption capacity fitted according to the Langmuir model was 445.29 mg/g, exceeding those of most previous chitosan-based adsorbents. The major reaction mechanism involving the capture and reduction of Cr(VI) has been systematically investigated based on FTIR, XPS and DFT analyses. Particularly, the fixed-bed column experiments illustrated that the effective treatment volume of PCA was 36367 mL and 7453 mL in simulated chromium wastewater and real chromium wastewater with initial concentrations of 2 mg L−1 and 52.88 mg L−1, respectively, suggesting the promising potential of PCA for large-scale practical applications. More interestingly, the current aerogel adsorbents could significantly reduce the accumulation of heavy metal ions in wheats, which meant that heavy metal wastewater had great prospects for agricultural irrigation after being treated by the aerogel of this work. In summary, this strategy could provide valuable and promising contribution towards the development of scalable and sustainable chitosan-based aerogels for Cr(VI) removal from practical wastewater. [ABSTRACT FROM AUTHOR]