The isomer-selective properties of the carbon adsorbent Carbopack Y modified by successively applied immiscible monolayers of 4-n-octyloxy-4'-cyanobiphenyl mesogen and β-cyclodextrin have been studied. It has been shown that the bilayer modified adsorbent has a high selectivity to structural and optical isomers under the conditions of the gas-adsorption chromatography. Thermodynamic justification of the selectivity and its temperature dependence has been given. Compensation temperatures for the reversal of the isomer conversion from the chromatographic column have been calculated.