This chapter discusses the development of arc discharge method in organic solvents for the formation of DNA encapsulated carbon nanotubes. The arc discharge is performed using graphite electrodes in a DNA/distilled water and DNA/methanol solution, and as a result, the soot is obtained in the solution containing multi-walled carbon nanotubes and onion-like nanocarbons. The arc discharge is performed in a DNA/toluene solution, and the soot is obtained at the electrode tip. The contained nanomaterials have spheroidal shapes. This arc discharge method in the DNA dispersed solution has a possibility for formation of the encapsulation of DNA into their structure. The structural characterization of the soot is performed with field emission transmission electron microscopy (FE-TEM) and Raman spectroscopy. The spectroscopic features of the plasma emission during discharge are measured using optical emission spectroscopy (OES).