The lack of scalable synthesis of transition metal dichalcogenides, such as molybdenum disulfide (MoS2), has proved to be a significant bottleneck in realization of fundamental devices and has hindered the commercialization of these materials in technologically relevant applications. In this study, a cost-efficient and versatile thin-film fabrication technique based on ionized jet deposition (IJD), i.e., a technique potentially providing high processing efficiency and scalability, is used to grow MoS2 thin films on silicon substrates. The operating conditions of IJD were found to influence mainly the ablation efficiency of the target and only slightly the quality of the deposited MoS2 thin film. All as-deposited films show chemical properties typical of MoS2 with an excess of free, elemental sulfur that can be removed by post-deposition annealing at 300–400 °C, which also promotes MoS2 crystallization. The formation of an interface comprised of several silicon oxide species was observed between MoS2 and the silicon substrate, which is suggested to originate from etching and oxidizing processes of dissociated water molecules in the vacuum chamber during growth. The present study paves the way to further design and improve the IJD approach for TMDC-based devices and other relevant technological applications.