International audienceNanocrystalline CNx particles and thin films were produced in a flow reactor system by the CO2 laser pyrolysis of sensitised NH3-N2O-C2 H2reactant gas mixtures. Depending on the substrate nature (silicon or quartz) the SEM and TED analysis of the CNx thin films revealed specific nucleation and growth morphologies of crystallites, resembling the β-C3 N4 phase. In the case of C3 N4 nanopowder synthesis, the relative concentration of the sensitisers (SF6 /C2 H4 ) was varied to minimise SF6 decomposition. The majority of the data obtained from powder analysis (XRD, XPS, and ir transmission measurements) suggests the presence of CN bonded phases and the formation of α-and β-C3 N4 structures