In this paper coal, source has been used in place of graphite for synthesis of single-walled carbon nanotubes (SWCNTs) with new Zr/Ni bimetallic catalyst. Using coal as starting material to produce the high-value-added SWCNTs is an economically competent route. SWCNTs have been synthesized by the electric arc discharge method using the so-called heterogeneous annealed coal anode filled with Zr and Ni catalyst. SWCNTs have been synthesized using annealed coal rod. The SWCNTs bundles synthesized generally have diameters of 4-10 nm. Most of those produced with Zr/Ni as the catalyst has a diameter ranging from 2.0 to 1.0 nm. The as-synthesized SWCNTs have been characterized employing XRD, HRTEM, EDX, Raman spectroscopy, and FTIR. It has been found that the change of the ratio of Zr and Ni concentration (wt%) in the catalyst affects the yield of SWCNTs. However, the purity of SWCNTs is very sensitive to the concentration of Zr. An optimal range of Zr/Ni compositions for synthesis of SWCNTs with relatively high purity and yield is obtained at specific concentration of 3:1.