Three indigenous systems-the underwater arc discharge setup, the inert environment arc discharge system, and the chemical vapor deposition (CVD) system-for the gram-scale production of carbon nanotubes were designed and fabricated. In this study, a detailed description of the development and fabrication of these systems is given. Carbon nanotubes were synthesized by using all the three systems, and comparative analyses of the morphology, composition, and purity were done. The synthesized materials were characterized using scanning electron microscopy, X-ray diffraction (XRD), and Raman spectroscopy. The scanning electron microscopy images show agglomerated tubed fiberlike structures in samples from the arc discharge setup, whereas samples from the CVD system do not show any tubelike structures decorated around the carbon nanotubes. Structural investigations done using powder XRD revealed the presence of the hexagonal crystallographic phase. Furthermore, the presence of the G and 2D bands reveals sp hybridization and confirms the presence of carbon nanotubes in samples. In conclusion, carbon nanotubes synthesized via the CVD system is of high quality and quantity. Moreover, the CVD is a cheap, easy to operate, and energy-saving synthesis method compared with the other two methods.