Synthetic zeolite Na-X and clinoptilolite (Cp) as well as their modifications with quaternary ammonium,salts were used to remove volatile-organic compounds (VOCs) and polycyclic aromatic hydrocarbons (PAHs) from aqueous solutions. A novel procedure was developed for the synthesis of orgatio-zeolites which consisted of surface modification with hexadecyltrimethylammonium bromide (HDTMA) in amounts of 1:0 and 2:0 of external cation exchange capacity (ECEC). Modification of both zeolites with HDTMA improved sorption properties. p-Xylene and dibenz[a,h]anthracene were adsorbed in amounts of 6.82 and 0.65 mg/g, respectively. Ethylbenzene and naphthalene were the lowest-removed hydrocarbons (2:99 and 0.058, respectively): The removal efficiencies for BTEX followed the order p-xylene > toluene > benzene > ethylbenzene, and for PAHs they followed the order dibenz[a,h]anthracene > benzo[a]pyrene > anthracene > naphthalene. Efficiency of sorption depends on-the-chemical properties of the various, organic compounds (dipole moment, molar mass, molecule structure, and the time of the sorption process) and zeolites properties, like the Si/Al ratio, texture parameters, particle size, and external cation exchange capacity. The mechanism of the sorption consists of dissolving the VOCs and PAHs into: the organic layer of the surfactant as well as on the penetration of organic solution into the mesopores.