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[Display omitted] • Elastic brushite/polyethyleneimine/nanofibrillated cellulose aerogel was developed. • The coupling of brushite and polyethyleneimine enhanced adsorption property. • PNFCA/BRU-0.2 exhibited high selectivity for Cu(II) with 332.66 mg/g. • The continuous flow purification of copper-containing wastewater was realized. • PNFCA/BRU-0.2 could block the toxicity of heavy metals to crops. To achieve efficient removal of copper(II) from heavy metal wastewater, designing an eco-friendly and low-cost adsorbent is highly desirable. Here, a novel air- and underwater shape-memory cellulose aerogel was reported via coupling brushite and polyethyleneimine (PEI)-modified nanofibrillated cellulose (NFC) for selectively adsorbing Cu(II) ions. The adsorption kinetic and isotherm studies were consistent with pseudo-second-order model and Langmuir model, indicating the removal of Cu(II) was a monolayer chemisorption process. Benefiting from the open three-dimensional (3D) framework structure and abundant exposed active sites, such compressible aerogel exhibited excellent adsorption capacity of 332.66 mg/g for Cu(II). In addition, the developed aerogel could be conveniently used as a continuous flow filter for successive purification of industrial wastewater, where the up-to-standard treatment volume was about 5.6 L. The Cu(II)-loaded aerogel could be regenerated after being eluted by 0.1 M EDTA-2Na, and its structure, shapeability and selective adsorption properties were hardly affected even after 8 consecutive cycles. Mechanistic analysis confirmed that the surface complexation, ion exchange and chemical deposition were the main driving forces for the superior adsorption performance. Finally, PNFCA/BRU could inhibit the contamination of crops by heavy metals, which was a great safeguard for wheat growth. [ABSTRACT FROM AUTHOR]