The functionalization of cellulose nanocrystal (CNC) aerogels was achieved through a two-step synthetic procedure. CNC aerogels were prepared under hydrothermal conditions, followed by solvent exchange and critical point drying. The CNC aerogels were functionalized with a methacrylate group and then underwent thiol-ene click chemistry to impart a range of functionalities onto the surface of the CNC aerogel. The use of the functionalized aerogels as oil absorbents was then investigated, with the most hydrophobic CNC aerogel, 1H,1H,2H,2H-perfluorodecanethiol-functionalized CNC aerogel, exhibiting the highest absorption of xylenes at 2.9 mL g(-1).