During the recent years, considerable attention has been given to the development of efficient and environmentally friendly technologies for the production of ceramic matrix composites. However, little research has been carried out on use of methylsilane (MS) as a halogen‐free precursor in the CVI process. The goal of this work was therefore to study the production of SiC‐matrix composites by pulse chemical vapor infiltration (PCVI) method with MS as a precursor and recently developed organomorphic frameworks as preforms. Experimental research was combined with numerical modeling to get deeper insight into the physical mechanisms underlying the technological process. Results of the study demonstrated that the PCVI allows performing the process with higher densification rate compared to continuous‐flow modifications of CVI. It is shown that optimization of PCVI providing a compromise between the utilization efficiency of the precursor, the densification uniformity, and the process time requires a proper choice of duration of the deposition stage and the process temperature. Numerical modeling proved to be a helpful tool in research and development of PCVI technology.