AbstractThe ongoing miniaturization of electronic devices has boosted the development of new post-silicon two-dimensional (2D) semiconductors, such as transition metal dichalcogenides, one of the most prominent materials being molybdenum disulfide (MoS₂). A major obstacle for the industrial production of MoS₂-based devices lies in the growth techniques. These must ensure the reliable fabrication of MoS₂ with tailored 2D properties to allow for the typical direct bandgap of 1.9 eV, while maintaining large-area growth and device compatibility. In this work, we used a versatile and industrially scalable MoS₂ growth method based on ionized jet deposition and annealing at 250 °C, through which a 3D stable and scalable material exhibiting excellent electronic and optical properties of 2D MoS₂ is synthesized. The thickness-related limit, i.e., the desired optical and electronic properties being limited to 2D single/few-layered MoS₂, was overcome in the thin film through the formation of encapsulated highly crystalline 2D MoS₂ nanosheets exhibiting a bandgap of 1.9 eV and sharp optical emission. The newly synthesized 2D-in-3D MoS₂ structure will facilitate device compatibility of 2D materials and confer superior optoelectronic device function.