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[Display omitted] • A functionalized carboxymethyl chitosan aerogel is explored for Cu(Ⅱ) adsorption. • The maximum capacity of PCCSA-1.0 for absorbing Cu(Ⅱ) is 175.56 mg/g. • Continuous filtration of industrial wastewater with fixed bed columns is achieved. • PCCSA-1.0 is conducive to inhibit the enrichment of Cu(Ⅱ) ions in rice. • The generated waste after adsorption is converted into a material for secondary use. Copper ions (Cu(II)) in water pose a huge threat to human health and ecosystem security. Therefore, developing eco-friendly and sustainable strategies to eliminate the toxicity risk of Cu(II) in the aqueous environment remains a great challenge. In this work, an elastic polyethyleneimine-modified carboxymethyl chitosan aerogel was developed via a freeze-drying process for the adsorption of Cu(II). The adsorption kinetic and isotherm experiments demonstrated that the adsorption process was monolayer chemisorption and the maximum adsorption capacity calculated from Langmuir model was 175.56 mg g−1. The obtained aerogels exhibited preferential selectivity for Cu(II) even when the competing cations and organics existed. Besides, about 0.93 g of aerogel realized continuous fixed-bed column filtration of industrial wastewater with an effective purification volume of 4.14 L. Mechanistic analysis via FTIR and XPS revealed that the excellent adsorption performance for Cu(II) might be attributed to the strong electrostatic force, Vander Waals' force and coordination of N/O -containing functional groups. It is worth mentioning that the adsorbed Cu(II) ions in the aerogel were converted into a reusable photocatalyst, avoiding the secondary leakage of heavy metals. This work opened a door to synthesize carboxymethyl chitosan aerogel, promising for heavy metal wastewater treatment and realizing the concept of waste utilization. [ABSTRACT FROM AUTHOR]