Atmospheric pressure plasma jets (APPJ) are widely used in industry for surface cleaning and chemical modification. In the recent past, they have gained more scientific attention especially in the processing of carbon nanomaterials. In this work, a novel power generation technique was applied to realize the stable discharge in N2 (10 vol.% H2) forming gas in ambient conditions. This APPJ was used to reduce solution-processed graphene oxide (GO) thin films and the result was compared with an established and optimized reduction process in a low–pressure capacitively coupled (CCP) radiofrequency (RF) hydrogen (H2) plasma. The reduced GO (rGO) films were investigated by Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). Effective deoxygenation of GO was observed after a quick 2 s treatment by AAPJ. Further deoxygenation at longer exposure times was found to proceed with the expense of GO–structure integrity. By adding acetylene gas into the same APPJ, carbon nanomaterials on various substrates were synthesized. The carbon materials were characterized by Raman spectroscopy, scanning electron microscopy (SEM), and energy-dispersive X-ray (EDX) analyses. Fullerene-like particles and graphitic carbon with short carbon nanotubes were detected on Si and Ag surfaces, respectively. We demonstrate that the APPJ tool has obvious potential for the versatile processing of carbon nanomaterials.