Highly ordered C-60 layers prepared on mica and HOPG (highly ordered pyrolytic graphite) substrates by physical vapour deposition were nanostructured by different electrochemical procedures using ionic liquid (1-butyl-3-methyl-imidazolium tetrafluoroborate) as electrolyte. The topology of the films is completely changed and a tenfold larger cluster size than in aqueous solutions was obtained. The most homogeneous films were obtained when lithium trifluoromethanesulfonate was added to the ionic liquid. FTIR spectroscopy was used to study the molecular structure of the nanostructured fullerene films. (C) 2004 Published by Elsevier Ltd.