The supramolecular nanoarchitectures, C-60/ferrocene nanosheets, were prepared by a simple liquid-liquid interfacial precipitation method and fully characterized by means of SEM, STEM, HRTEM, XRD, Raman and UV-vis-NIR spectra. The highly crystallized C-60/ferrocene hexagonal nanosheets had a size of ca. 9 mu m and the formulation C-60(ferrocene)(2). A strong charge-transfer (CT) band between ferrocene and C-60 was observed at 782 nm, indicating the presence of donor-acceptor interaction in the nanosheets. Upon heating the nanosheets to 150 degrees C, the CT band disappeared due to the sublimation of ferrocene from the C-60/ferrocene hybrid, and C-60 nanosheets with an fcc crystal structure and the same shape and size as the C-60/ferrocene nanosheets were obtained.