Deposition of thin SiC x N y layers from a new single-source organosilicon compound, methyltris(diethylamino)silane (MTDEAS) mixed with helium or nitrogen is studied by using thermodynamic simulation of Si-C-N-H(He)-O system and experimentally by low pressure (10 −2 -10 Torr) plasma enhanced chemical vapor decomposition (PECVD) in the temperature range of 300-1300 K. Thermodynamic simulation allowed to find the temperature boundaries of solid phase formation. The phase composition, as well as physicochemical and functional properties of the layers has been studied using a complex of modern experimental techniques, including Raman spectroscopy, scanning electron (SEM) and atomic force microscopy (AFM), X-ray diffraction using synchrotron radiation (XRD-SR), ellipsometry and spectrophotometry. The electrophysical parameters were measured using the C-V characteristics. The microhardness and Young's modulus were determined by Nanoindentation method. It was shown that the layers contain crystals of phases belonging to Si 3-x C x N 4 structures, such as α-Si 3 N 4 , α-Si 2 CN 4 , α-SiC 2 N 4 , and α-C 3 N 4 which, possibly, are embedded in the amorphous matrix of silicon carbonitride layers.