The aim of this chapter is to report the results on synthesis DLC thin films and carbon nanocomposites by the versatile nanofabrication method based on plasma entitled thermionic vacuum Arc TVA . TV" technology is based on the localized ignition of the arc plasma in vacuum conditions. "mong thin film coating methods by vacuum deposition techniques with high purity, low roughness, and good adhesion on the substrates, TVA is one of the major suitable methods to become a powerful coating technology. Two or three different TV" discharges can be ignited simultaneously in the same chamber for multi-material processing using TV" and separate power supplies. These TV" discharges are localized and do not interfere with each other. Simultaneous two or three TV" discharges were already used for the production of alloy/composite of various materials. This is due to the high versatility concerning the configuration of experimental arrangements, taking into account the number of electron guns, symmetry of the electrodes, relative position of the anode versus cathode, and also the huge opportunity to combine the materials to be deposited bi-and multi-layers, nanocomposites, or alloys in order to have specific applications. This chapter presents the comparative results concerning the surface-free energy information processing, the reflective index, the hardness, and the morphology to provide a coherent description of the diamond-like carbon films and carbon nanocomposites synthesized by thermionic vacuum arc TV" and related configurations where Me = "g, "l, Cu, Ni, and Ti: binary composites CMe, C-Si and ternary composites C+Si+Me . The results include reports on the distribution in size, surface, geometry, and dispersion of the nanosized constituents, tailoring and understanding the role of interfaces between structurally or chemically dissimilar phases on bulk properties, as well as the study of physical properties of nanocomposites structural, chemical, mechanical, tribological . The results presented