Natural alpha-, beta-, and gamma-cyclodextrins (CDs) were intercalated in the interlayer of layered double hydroxide (LDH) by calcination-rehydration reaction using the calcined precursor of Mg-Al/CO3/LDH. The intercalated amount was considerably large in spite of nonanionic macrocyclic molecule in the wide CD concentration range. The presence of hydroxyl group on upper and lower rim in CD molecule favors the intercalation driving force by hydrogen bond with the hydroxide basal layer. In addition, CDs in the CD/LDHs were deintercalated by the ion exchange with carbonate ion with regeneration of the pristine Mg-Al/ CO3/LDH.