To produce novel thin-film spintronic materials based on a thermodynamic simulation, condensed phases with a complex composition are deposited in Si–С–N–H–M systems (M = Fe, Co, Ni) in a wide temperature range of 500-1300 K. As a result of the simulation CVD diagrams of Fe–Si–C–N–H(He), Co–Si–C–N–H(He), and Ni–Si–C–N–H(He) systems are obtained which enable the optimization of the synthesis process for film materials such as SiCxNyFez, SiCxNyCoz, and SiCxNyNiz. SiCxNyFez films are experimentally deposited from a gas mixture containing ferrocene (C5H5)2Fe, organosilicon compound 1,1,1,3,3,3-hexamethyldisilazane HNSi2(CH3)6 (HMDS) under reduced pressure in the temperature range 1073-1273 K. The dependence of the physicochemical and functional properties of SiCxNyFez films on the synthesis conditions is found by a comples of modern research techniques such as IR and Raman spectroscopy, EDS, XPS, SEM, HREM, and synchrotron radiation powder XRD (SR XRD). By the Faraday method and electron paramagnetic resonance (EPR) the magnetic properties of the films are analyzed. It is shown that at a synthesis temperature of 1123 K the films are paramagnetic, and at a higher deposition temperature of 1273 K they are ferromagnetic.