Graphene materials are synthesized in a thermal plasma jet without using size forming catalysts. The synthesis was performed on a direct current plasma torch operating at 28–30 kW with a pressure of 100–710 Torr. The synthesis products are studied by electron microscopy, X-ray diffraction, and dynamic light scattering. It is found that structures formed in the plasma jet have a flake morphology regardless of the type of the carbon bearing source. Thermodynamic calculations testify a correlation between the temperature profile in the plasma jet and the composition of condensed carbon (redistribution between C60 and C80). The application areas of flaky structures are discussed.