Mesoporous amorphous sodium-aluminosilicate host matrices of composition Si1−xAlxNaxO2, 0.1 ≤ x ≤ 0.33, obtained by sol-gel methodology, have been used as sequestrating agents for the cationic dye Rhodamine 6G (Rh6G) in solution. Favorable adsorption kinetics and a wide pH working range (4–10) as well as high sorption capacities for Rh6G render these materials potentially useful reagents for effective dye removal from wastewaters. While the experimentally realized sorption capacities fall significantly below the theoretical limits, used materials can be thermally re-cycled by pyrolizing the sequestrated dye molecules. Solid state NMR and BET measurements show that this process occurs under preservation of the materials' structural integrity, allowing it to be re-used multiple times.