Molecular layer deposition (MLD) of thin polyamide films was performed using 1,3,5-benzenetricarbonyltrichloride (trimesoyl chloride, TMC) and 1,2-ethylenediamine (EDA) as precursors at a temperature of 120°С. The growth rate at this temperature was 1.85 nm/cycle. In situ quartz crystal microbalance (QCM) study was used to determine the film growth behavior. QCM signal showed linear film growth with an increasing number of MLD cycles. Pyrolysis of MLD polyamide films on Si(111) was conducted at temperatures of 1100 and 1300°С and a pressure of 10−7 Torr. Thin heteroepitaxial films of β-SiC (3C–SiC) on the Si(111) were obtained as a result of a solid-phase reaction between Si and C at 1300°С. A variety of high-resolution spectroscopic techniques were used to determine the elemental composition and crystal structure of organic and ceramic films.