The theoretical simplicity of sp 2 carbons, owing to their having a single atomic type per unit cell, makes these materials excellent candidates in quantum chemical descriptions of vibrational and electronic energy levels. Theoretical discoveries, associated with sp 2 carbons, such as the Kohn anomaly, electron-phonon interactions, and other exciton-related effects, may be transferred to other potential 2D materials. The information derived from the unique Raman bands from a single layer of carbon atoms also helps in understanding the new physics associated with this material, as well as other two-dimensional materials. The following chapter describes our studies of the G, D, and G′ bands of graphene and graphite, and the characteristic information provided by each material. The G-band peak located at ~1586 cm −1 , common to all sp 2 carbons, has been used extensively by us in the estimation of thermal conductivity and thermal expansion characteristics of the sp 2 nanocarbon associated with single walled carbon nanotubes (SWCNT). Scanning electron microscope (SEM) images of functionalized graphene nanoplatelet aggregates doped with argon (A), carboxyl (B), oxygen (C), ammonia (D), fluorocarbon (E), and nitrogen (F), have also been recorded and analyzed using the Gwyddion software.