In aqueous solution, low charged polyoxometalates (POMs) exhibit remarkable self-assembly properties with non-ionic organic matter that have been recently used to develop groundbreaking advances in host-guest chemistry, as well as in soft matter science. Herein, we exploit the affinity between chaotropic POM and native cyclodextrins (α-, β-, and γ-CD) to enhance the structural and functional diversity of cyclodextrin-based open frameworks. At first, we reveal that the Anderson-Evans type polyoxometalate [AlMo6O18(OH)6] 3represents an efficient inorganic scaffold to design open hybrid frameworks built from infinite cyclodextrin channels connected through the disc-shaped POM. Single-crystal X-ray analysis demonstrates that the resulting supramolecular architectures contain large cavities (up to 2 nm) where the topologies are dictated by the rotational symmetry of the organic macrocycle, generating honeycomb-(bnn net) or checkerboards-like (pcu net) networks for α-CD (C6) or γ-CD (C8), respectively. On the other hand, the use of β-CD, a macrocycle with C7 ideal symmetry, led to a distorted checkerboard-like network. The cyclodextrin-based frameworks built from Anderson-Evans type POM are easily functionalizable using the molecular recognition properties of the macrocycle building units. As proof of concept, we successfully isolated a series of compartmentalized functional frameworks by the entrapment of poly-iodides or superchaotropic redox-active polyanions within the macrocyclic hosting matrix. This set of results paves the way for designing multifunctional supramolecular frameworks whose pore dimensions are controlled by the size of inorganic entities.