A plasma process for making cyanide from nitrogen and hydrocarbon (methane and propane) has been successfully demonstrated, which can directly fix atmospheric nitrogen into hydrocarbons. Nitrogen serves as both the plasma gas and the primary reactant. The thermodynamic analysis as well as the experimental outcome indicates that it is feasible to achieve very high conversion of hydrocarbons into cyanide by increasing the partial pressure of nitrogen gas within the reaction mixture, but the high conversion comes at a cost of an increase in total energy consumption and was detrimental to process energy efficiency. Hence, the process was optimized based on specific energy consumption (SEC) instead of conversion. The conversion with respect to nitrogen and hydrocarbon ratio follows thermodynamic prediction. The primary byproducts obtained were hydrogen, acetylene, and soot. The laboratory system was stable and could be run for extended periods, achieving a minimal SEC of approximately 15.5 kW h/kg NaCN.