The regularities of the dynamic solid-phase extraction of organic substances (exemplified by chloroform, butyl acetate, and diethyl ether) from aqueous solutions on composite surface-layer sorbents, in which a finely dispersed sorption-active carbon material (active carbon or nanocarbon) was supported onto the surface of porous polytetrafluoroethylene, were found. It was demonstrated that the efficiency of the sorbents developed was higher than that of traditional bulk porous sorbents used for the preconcentration of volatile organic substances from aqueous solutions.