The structure of the C60 and p-Bu(t)-calix[8]arene complex has been reinvestigated, showing an unprecedented continuous layered tetragonal array of fullerenes encapsulated by calixarenes. Electron diffraction data revealed the tetragonal symmetry, with a stepped structure observed by AFM and SEM, and the thickness of the basal plane was measured by XRD, as 2 nm. The molecular simulated arrangement of fullerenes accounts for the ability to take up to ca. 11% of fullerenes C70 in place of the smaller fullerene.