C-60 molecules were incorporated into the interlayer of a layered Mg/Al double hydroxide compound, and the physicochemical properties of these spherical molecules arranged in two-dimensional arrays were examined. The precursor used was a double hydroxide with dodecyl sulfate counteranions. C-60 molecules were introduced by dissolving the molecules into the interlayer hydrophobic phase. After heating the resultant compound under vacuum to decompose the dodecyl sulfate, C-60 molecules were sandwiched in between the double hydroxide layers. The C-60-incorporated compounds were characterized with X-ray diffraction, thermal gravimetric analysis, and Raman, UV-vis, and solid state NMR spectroscopies. Among them, the most powerful technique to identify the environment of C-60 was solid State C-13 NMR. The results of T-1 relaxation time and fwhm line width measurement showed that the incorporated C-60 molecules did not rotate as freely as in the pure solid form and experienced rather intimate interactions with either the interlayer proton-containing species or the lattice atoms.