Dyes are widely used in different areas of industry and belong to the most important pollutants of water resources. Potential toxicity of dye molecules encourages the creation of effective materials for their concentration and removal. In the present work, a simple strategy was proposed for synthesis of β-cyclodextrin (CD)-containing silica adsorbent with hexagonally ordered mesoporous structure. In the first step, chemical modification of β-CD with (3-aminopropyl) triethoxysilane by use of 1,1'-carbonyldiimidazole as coupling agent was realized. Then synthesized β-CD-containing silane was involved into the co-condensation reaction with tetraethyl orthosilicate in the presence of template – quaternary alkylammonium ionic surfactant. Effect of reaction medium composition used in synthesis of functional silane on chemical and porous structure of βCD-containing silica materials was elucidated by IR spectral and chemical analysis of surface functional groups as well as low-temperature adsorption-desorption of nitrogen and x-ray diffraction analysis. Adsorption of methyl red (MR) by parent MCM-41 and synthesized -CD-silica was studied in dependence of solution acidity and equilibrium concentration of dye in phosphate buffer solutions. 0.00 0.04 0.08 0.12 0.16 0.00 0.02 0.04 0.06 0.08 0.10 pH 1.0 A (mol/m2) Ceq (mmol/l) 0.00 0.04 0.08 0.12 0.16 0.00 0.02 0.04 0.06 0.08 0.10 pH 7.0 A (mol/m2) Ceq (mmol/l) a b Figure. Isotherms of MR adsorption on MCM-41 (○) and -CD-MCM-41 (■) silicas. It was found that incorporation of cyclic oligosaccharide moieties into the hexagonally arranged mesoporous framework leads to the enhancement of adsorption efficiency towards MR. To elucidate mechanism of MR distribution between the liquid phase and silica adsorbent and optimize the design of an adsorption system for dye removal the equilibrium adsorption data were analyzed using four widely applied isotherm models: Langmuir, Freundlich, Redlich-Peterson, and BET. Error analysis showed that the Redlich-Peterson is the most appropriate for fitting the experimental data obtained for MR adsorption on -CD-silica at pH 1.0 and pH 7.0.