The outstanding characteristics of carbon nanotube (CNT) including structure, mechanical, optical, electric, and magnetic properties generate a great number of exciting possible applications. The influence of starting carbon materials on the synthesis of CNT is investigated. Comparisons are made between graphite rods and polycyclic aromatic hydrocarbon (PAR) as carbon source in helium arc discharge. The SEM micrographs of CNT deposits formed on the top surface of cathode show quasi-hexagonal structure. The column structures of CNT along the deposition axis of graphite rod approximately are seen in the cross-section of specimen. The fine columnar structure consists of randomly oriented fiber-like CNTs. HRTEM image clearly shows the characteristic feature of multi-walled CNT. CNT core is hollow with multiple layers parallel to CNT axis on the wall. PAH can serve as building blocks for CNT formation. The high temperature graphitization process induced by the arc plasma enables the hydrocarbons acted as carbon sources and changes the aromatic species into the layered graphitic structure of CNT.