This paper discusses the influence of the structure of copolymers based on glycidyl methacrylate and alkyl methacrylates with C6–C18 hydrocarbon side groups on the wettability and sorption properties of surface-modified chitosan aerogels. The grafting of copolymers onto the surface of aerogels was confirmed by elemental analysis, X-ray photoelectron spectroscopy, and Fourier-transform infrared spectroscopy. As a result of the modification, with an increase in the amount of the hydrocarbon substituent alkyl methacrylate, the surface of the resulting materials became hydrophobic with contact angles in the range of 146–157°. At the same time, the water absorption of the aerogels decreased by a factor of 30 compared to that for unmodified aerogels, while the sorption capacity for light oil, diesel fuel, and synthetic motor oil remained at the level of more than 30 g/g. Chitosan aerogels with grafted copolymers based on glycidyl methacrylate and alkyl methacrylates retain biodegradation capacity; however, compared to unmodified chitosan, this process has an induction period.