Three different polysaccharides, xanthan gum, chitosan and locust bean gum, were crosslinked with or without ß-cyclodextrin, using citric acid in different ratios, to create "green" hydrogel matrices. The crosslinking of these polysaccharides was produced through an inexpensive and innocuous solvent-free synthesis process. A favorable swelling behavior of the hydrophilic matrices facilitates the sorption of the solutes tested. Interestingly, the amount of ß-cyclodextrin groups is not the only factor to yield the best sorption capability for hydrophobic model molecules: polysaccharides themselves also influence the sorption depending on their characteristic functional groups, the conformation of their chains and, as mentioned above, their degrees of swelling. In order to ascertain the effect of the polysaccharides on the sorption capabilities of a model sorbate (1-naphthol), isotherms using a wide range of solute concentrations were analyzed, and the Hill equation yielded the best fitting results and provided some insight into the mechanisms of interaction.