?-Cyclodextrin can assemble in the presence of KOH or RbOH into metal-organic frameworks (CD-MOFs) with applications in gas adsorption and environmental remediation. Crystalline CD-MOFs are grown by vapor diffusion and their reversible adsorption of CO[subscript 2](g) is analyzed both qualitatively and quantitatively. The experiment can be tailored to high school through advanced undergraduate laboratories and engages students in several areas of fundamental chemistry (crystallization, chemical equilibria, acid-base reactions, gas laws), advanced materials (MOFs), and broader impacts of chemistry (renewable resources and environmental chemistry).