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Two‐dimensional (2D) transition metal dichalcogenides (TMDCs) with unique electrical properties are fascinating materials used for future electronics. However, the strong Fermi level pinning effect at the interface of TMDCs and metal electrodes always leads to high contact resistance, which seriously hinders their application in 2D electronics. One effective way to overcome this is to use metallic TMDCs or transferred metal electrodes as van der Waals (vdW) contacts. Alternatively, using highly conductive doped TMDCs will have a profound impact on the contact engineering of 2D electronics. Here, a novel chemical vapor deposition (CVD) using mixed molten salts is established for vapor–liquid–solid growth of high‐quality rhenium (Re) and vanadium (V) doped TMDC monolayers with high controllability and reproducibility. A tunable semiconductor to metal transition is observed in the Re‐ and V‐doped TMDCs. Electrical conductivity increases up to a factor of 10 8  in the degenerate V‐doped WS 2  and WSe 2 . Using V‐doped WSe 2  as vdW contact, the on‐state current and on/off ratio of WSe 2 ‐based field‐effect transistors have been substantially improved (from ≈10 –8  to 10 –5  A; ≈10 4  to 10 8 ), compared to metal contacts. Future studies on lateral contacts and interconnects using doped TMDCs will pave the way for 2D integrated circuits and flexible electronics.

Tunable Doping of Rhenium and Vanadium into Transition Metal Dichalcogenides for Two‐Dimensional Electronics