Abstract: A method to obtain composite sorbents based on multilayer carbon nanotubes and AEROSIL has been developed, including mechanochemical treatment and gelation. The sorbents have been characterized by means of scanning electron microscopy, thermogravimetry, and adsorption methods. Multilayer carbon nanotubes have been fixed in a silica matrix, retaining their individuality; the synthesized sorbents have exhibited a mesoporous structure with developed surface. The nanocomposites based on carbon nanotubes with specific surface area of 200–270 m²/g can be efficient sorbents for the isolation of pure C₇₀ fullerene and the concentrating of volatile organic compounds.