In this work, we demonstrate plasma-catalytic synthesis of hydrogen and acrylonitrile (AN) from CH₄ and N₂. The process involves two steps: 1) plasma synthesis of C₂H₂ and HCN in a nominally 1:1 stoichiometric ratio with high yield up to 90% and high methane conversion > 90%; and 2) downstream thermocatalytic reaction of these intermediates to make AN. The effect of process parameters on product distributions and specific energy requirements are reported. If the catalytic conversion of C₂H₂ and HCN in the downstream thermocatalytic step to AN were perfect, which will require further improvements in the thermocatalytic reactor, then at the maximum output of our 1 kW radiofrequency 13.56 MHz transformer, a specific energy requirement of 73 kWh kgAN^-1was determined. The expectation is that scaling up the process to higher throughputs would result in decreases in specific energy requirement into the predicted economically viable range less than 10 kWh kgAN^-1.