High silica faujasite (FAU) and its hexagonal analog (EMT) were synthesized using 15-crown-5 and 18-crown-6, respectively, as templating agents. By mixing these two crown-ethers in the starting hydrogel, a material with a crystal morphology resulting from an overgrowth of both cubic and hexagonal structures was obtained. These three zeolites with a Si/Al molar ratio close to 4 were ion-exchanged and transformed into their protonated forms. The samples were characterized by chemical analysis, Si-29, Al-27, and Na-23 solid-state MAS n.m.r., and it was shown that the sodium removal was more complete in the hexagonal and overgrown samples. The acidity (determined by STD of ammonia) and the catalytic activity (evaluated by n-heptane cracking) are closely related to the residual amount of Na+, and they proved to be higher for the two latter samples.