LAUSR

Monolayer MoS2 has attracted significant attention owing to its excellent performance as an n‐type semiconductor from the transition metal dichalcogenide (TMDC) family. It is however strongly desired to develop controllable synthesis methods for 2D p‐type MoS2, which is crucial for complementary logic applications but remains difficult. In this work, high‐quality NbS2–MoS2 lateral heterostructures are synthesized by one‐step metal–organic chemical vapor deposition (MOCVD) together with monolayer MoS2 substitutionally doped by Nb, resulting in a p‐type doped behavior. The heterojunction shows a p‐type transfer characteristic with a high on/off current ratio of ≈104, exceeding previously reported values. The band structure through the NbS2–MoS2 heterojunction is investigated by density functional theory (DFT) and quantum transport simulations. This work provides a scalable approach to synthesize substitutionally doped TMDC materials and provides an insight into the interface between 2D metals and semiconductors in lateral heterostructures, which is imperative for the development of next‐generation nanoelectronics and highly integrated devices.