Abstract An efficient heavy metal adsorbent from quaternary ammonium-functionalized cellulose nanofiber aerogels was successfully developed. The highly porous aerogel could well retain its large specific surface area, which allowed rapid and effective removal of Cr(VI) from contaminated water. The aerogel adsorbent became mechanically robust after chemical crosslinking. It could be easily separated from water after adsorption without complicated centrifugation or filtration process. With only 1g of aerogel, more than 99% of Cr(VI) in 1L of 1mg/L solution could be removed in 50min. Besides, the aerogel also exhibited excellent reusability.