Carbon nanotubes (CNTs) are materials of interest in many fields of science and technology because of their remarkable electronic, mechanical, and thermal properties.[1] Soluble CNTs [2] and CNT-polymer nanocomposites, including CNT-DNA (RNA), possess unique superstructures. [3] It is known that patterned carbon nanotubes are formed on prepatterned substrates or prepatterned catalysts during the synthesis of carbon nanotubes. [4] Jiang and co-workers [5] reported the selfassembly formation of large-scale micropatterns on aligned multiwalled carbon nanotubes by the aid of the capillary action of water. Very recently, Li et al. [6] and Zheng and coworkers [7] described polymer-crystallization-driven periodic patterning on CNTs and controlled two-dimensional patterns of spontaneously aligned CNTs from DNA-wrapped CNTs on a SiO 2 surface. We now report the discovery that self-assembly of single-walled CNTs (SWNTs) with a honeycomb structure is spontaneous on solid substrates by simple solution casting of a SWNT-lipid conjugate (complex 1). Since the first report by François and co-workers [8] that selforganized honeycomb structures are formed from star-shaped poly(styrene) or poly(styrene)-poly(paraphenylene) block copolymers in carbon disulfide under flowing moist gas, considerable attention has focused on this area; that is, such superstructures are formed from the solution casting of: i) symmetric diblock copolymers, [9] ii) rod-coil diblock copolymers, [10] iii) a coil-like polymer, [11] iv) ion-complexed polymers, [12] lipid-packaged Pt complexes, [13] v) poly(D,L-lactic-co-glycolic acid), [14] and vi) polysulfone.[15]As shown in Figure 1, complex 1 was easily obtained by the so-called polyion-complexed method; [16] that is, the mixing of an aqueous solution of shortened-SWNTs (s-SWNTs-COO -Na + ) and molecular bilayers of tridodecylmethylammonium chloride (3 C 12 N + Cl -) [17] in water produced a precipitate, which was collected to obtain complex 1. Mioskowski and coworkers [18] used lipids to dissolve CNTs in water; they described the formation of a supramolecular assembly of the lipids-multiwalled CNTs. The Raman spectra of the s-SWNTs and complex 1 were virtually identical (see Fig. S1 in the Supporting Information). The thermogravimetric analysis (TGA) curve (data not shown) of complex 1 revealed that the composition ratio, s-SWNTs/3 C 12 N + , was roughly 1:1 (w/w). Complex 1 was insoluble in water and in organic solvents, such as alcohols, acetone, and ethyl acetate, but soluble in several organic solvents including dichloromethane, chloroform, benzene, and toluene. In Figure 1, photographs of complex 1 and s-SWNTs-COOH only in chloroform are shown (for photographs in other solvent systems, see Fig. S2 in the Supporting Information). It is clear that complex 1 produces a transparent black solution/dispersion in the solvent. The asymmetric and symmetric methylene stretching vibrations in the Fourier transform infrared (FTIR) spectrum of a cast film of complex 1 appeared at 2924 and 2854 cm -1 , respect...