A very exceptional effect of pressure-induced dissolution has been revealed for an edible metal-organic framework, γ-CD-MOF-1, formed using γ-cyclodextrin and KOH base. In addition, a new polymorph of γ-CD-MOF-1 has been obtained. The trigonal structure is a symmetry sub-group modification of the cubic form. The pressure-induced dissolution of γ-CD-MOF-1 and its polymorphism are shown to be closely related and regulated by adsorption in the pores, as well as the guest framework interactions.