Lamellar nanowires with small tilt angle defects, epitaxially aligned along the lattice of highly oriented pyrolytic graphite (HOPG), have been constructed by spin-coating of a solution of a fullerene derivative covalently bearing double long-alkyl chains and characterized by atomic force microscopy (AFM) under ambient atmosphere. The small tilt angle defects in domains of lamellar assemblies are rarely found in nano-organized structures on HOPG due to the high 2D crystallinity of their long aliphatic chains in the lamellae. The distance between adjacent nanowires and the 2D crystallinity can be regulated by tuning the substituent pattern of the fullerene derivatives. Here, we also describe lamellar nanowire formation of a newly isolated fullerene bis-adduct bearing long alkyl chains. (C) 2007 Elsevier B.V. All rights reserved.