“…Theconstruction of conjugated p-systems on unique hexagonal networks of sp 2 -hybridized carbon atoms has been demonstrated, producing nanocarbon models with discrete structures. [12][13][14] Synthetically,afew examples of pentagon-embedded nanohoops have been realized in forms of heteroaromatic curved p-systems, [15][16][17][18][19] but the incorporation of pentagons into the curved conjugated systems of cylinder-shaped molecules with sp 2 -carbon networks has not been achieved. [3,4] In contrast, odd-numbered polygonal rings, such as pentagons and heptagons,a re much less explored in nanocarbon structures.Although pentagons and/or heptagons were initially perceived as structural defects that distort the nanocarbon shapes, [5][6][7][8][9] recent theoretical investigations indicate that odd-numbered rings could also give rise to flat or curved nanocarbon sheets through anomalous periodic arrangements.F or instance,p entagon/heptagon-containing cylinders of sp 2 -carbon networks,s uch as pentaheptite and haeckelite (Figure 1), [10,11] have been proposed, and their unique conjugated systems with enhanced metallic character have been extensively discussed in the context of novel tubular nanocarbon materials.Avariety of cylinder-shaped nanocarbon structures are currently being exploited to dramatically expand the theoretical models of cylindershaped nanocarbons with odd-numbered rings.…”