Abstract: Templated (T) and non-templated (NT) cross-linked materials containing β-cyclodextrin (β-CD) and epichlorohydrin (EPH) were prepared at variable β-CD: EPH ratios (1:15, 1:20, and 1:25) in the presence and absence of a molecular template (toluene). The structural characterization of the materials was carried out using spectroscopy (FT-IR, solids 13C NMR, and SEM) and thermogravimetric analysis (TGA). The adsorption properties were studied with phenol-based adsorbates (TNP; 2,4,6-trinitrophenol and PNP; p-nitrophenol) at equilibrium and dynamic conditions. The monolayer adsorption capacity (Qm) varied for the T-polymer/TNP systems (Qm = 0.10 to 0.95 mmol/g), and NT-polymer/TNP systems (Qm = 0.23 to 0.83 mmol/g). The range of Qm values for the T-polymer/ PNP systems (0.26 to 0.62 mmol/g) exceeded that of the NT-polymer/ PNP systems (0.23 to 0.40 mmol/g). The kinetic uptake profiles for the polymers and phenolphthalein (phth) are reliably described by the pseudo-first order (PFO) model. The β-CD inclusion site accessibility for the polymers varied from 15-20 %, according to the level of cross-linking, where the accessibility of the T-polymers was greater than the NT-polymers. The structural characterization and phenol adsorption properties provide complementary support for the role of tunable polymer morphology in adsorption processes. The role of two-site binding is demonstrated for linear and globular polymer materials according to the unique adsorption properties with phenols of variable size and hydrophile-lipophile character