A cost-effective and potentially industrially scalable, in situ functionalization procedure for preparation of soluble graphene nanoribbon (GNRs) from commercially available carbon nanotubes is presented. The physical characteristics of the functionalized product were determined using SEM, evolved gas analysis, X-ray diffraction, solid-state (13)C NMR, Raman spectroscopy, and GC-MS analytical techniques. A relatively high preservation of electrical properties in the bulk material was observed. Moreover, replacement of intercalated potassium with haloalkanes was obtained. While carbon nanotubes can be covalently functionalized, the conversion of the sp(2)-hybridized carbon atoms to sp(3)-hybridized atoms dramatically lowers their conductivity, but edge functionalized GNRs permit their heavy functionalization while leaving the basal planes intact.