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In this work, cellulose nanocrystals (CNCs) obtained by the acid hydrolysis of waste bamboo powder were used to synthesize cellulose nanocrystal-g-poly(acrylic acid-co-acrylamide) (CNC-g-P(AA/AM)) aerogels via graft copolymerization followed by freeze-drying. The structure and morphology of the resulting aerogels were characterized by Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM), and the CNC-g-P(AA/AM) aerogels exhibited excellent absorbent properties and adsorption capacities. Subsequent Pb(II) adsorption studies showed that the kinetic data followed the pseudo-second-order equation, while the adsorption isotherms were best described using the Langmuir model. The maximum Pb(II) adsorption capacity calculated by the Langmuir model reached up to 366.3 mg/g, which is a capacity that outperformed that of the pure CNC aerogel. The CNC-g-P (AA/AM) aerogels become structurally stable through chemical cross-linking, which enabled them to be easily regenerated in HCl solution and retain the adsorption capacity after repeated use. The aerogels were found to maintain 81.3% removal efficiency after five consecutive adsorption&ndash, desorption cycles. Therefore, this study demonstrated an effective method for the fabrication of an aerogel adsorbent with an excellent reusability in the effective removal of Pb(II) from aqueous solutions.