The adsorption of four common volatile organic compounds (VOCs), namely 1,1,1-trichloroethane, trichloroethylene, methanol and propanone, was studied by the gravimetric method in different cationic forms of Y zeolite and in pillared interlayered clays (PILCs). The latter were pillared with aluminium or zirconium oxide pillars using as starting materials two types of clays: a natural smectite and a synthetic laponite. In this way the adsorption of VOCs was studied in solids with different types of porosity, since zeolites and pillared smectites were mainly microporous materials, but the pillared laponites had a high proportion of mesoporous volume. Therefore, the adsorption isotherms of the VOCs in the zeolites and PILCs were mainly of type I, according to the IUPAC classification, but in the case of the pillared laponites type II isotherms were found. The absolute values of the amounts of VOCs adsorbed in the zeolites were about three times higher than for the pillared smectites. In the case of the pillared laponites the amounts adsorbed approached those of the pillared smectites in the region of the low relative pressures and, at the higher relative pressures, approached or in some cases exceeded the amounts adsorbed in Y zeolites. The adsorption isotherms were analysed by the Langmuir and the Dubinin–Astakhov equations. The latter was able to reproduce the experimental data and made possible the partial definition of a characteristic curve of adsorption. For the microporous solids the results showed that the adsorption of VOCs is favoured in those materials where the unspecific interactions can be expected to predominate, but the results obtained with the pillared laponites indicated that mesoporous materials also have a potential in the adsorption of VOCs.