The structural analyses of the graphene-based materials using Raman spectroscopy and TPD techniques complement each other. The Raman spectra can be used to investigate the concentration of surface defects such as SW and point defects. The TPD technique is suitable for analyzing the concentration of defects at the edges and adatoms of carbon materials, based on the detection of evolved gases such as H2, H2O, CO, and CO2. Further investigation using Raman spectroscopy coupled with the direct observation of defects by high-resolution TEM will be a powerful means of exploring more sophisticated materials.