Results of experimental study of the one-step plasma-based process of the synthesis of unsupported graphene and hydrogenated graphene are presented. A direct current (DC) plasma torch is used, the pressure is held at 350 Тоrr, and the flow rates of plasma forming gas (helium) and carbon source (propane-butane mixture) are kept constant. An influence of reactor geometry on the properties of synthesized product is investigated. Graphene and hydrogenated graphene were synthesized in an appreciable rate in the plasma jet volume under equal conditions using cylindrical and conical reactors accordingly. Synthesized graphene materials are characterized using electron microscopy, Raman spectroscopy, x-ray, and XPS analysis, confirming the existence of graphene and of hydrogenated graphene (graphane). In order to examine an influence of input parameters on the process of the synthesis of graphene materials, the quasi-1D numerical flow model is used to calculate the distributions of temperature and velocity within the reactor channel. The key role of the temperature distribution within the reactor in the synthesis of graphene materials is established. Cylindrical flow channel provides higher temperatures compared with the conical channel. It affects the flow composition at the outlet. Under lower temperature, the flow contains in addition to condensed carbon a great amount of hydrocarbons CH, which is favorable for the production of hydrogenated graphene. Under higher temperature, the pure graphene is synthesized, since the outlet flow has the carbon mainly in the condense phase, the quantity of CH being insignificant.