Although fullerenes were discovered nearly 35 years ago, scientists still struggle to isolate "single molecule" tubular fullerenes larger than C 90 . In similar fashion, there is a paucity of reports for pristine single-walled carbon nanotubes (SWNTs). In spite of Herculean efforts, the isolation and properties of pristine members of these carbonaceous classes remain largely unfulfilled. For example, the low abundance of spherical and tubular higher fullerenes in electric-arc extracts (<0.01−0.5%) and multiplicity of structural isomers remain a major challenge. Recently, a new isolation protocol for highly tubular f ullerenes, also called f ullertubes, was reported. Herein, we describe spectroscopic characterization including 13 C NMR, XPS, and Raman results for purified [5,5] fullertube family members, D 5h -C 90 and D 5d -C 100 . In addition, DFT computational HOMO−LUMO gaps, polarizability indices, and electron density maps were also obtained. The Raman and 13 C NMR results are consistent with semiconducting and metallic properties for D 5h -C 90 and D 5d -C 100 , respectively. Our report suggests that short [5,5] fullertubes with aspect ratios of only ∼1.5−2 are metallic and could exhibit unique electronic properties.