Monolayers of transition metal dichalcogenides (TMDCs) have attracted a great interest for post‐silicon electronics and photonics due to their high carrier mobility, tunable bandgap, and atom‐thick 2D structure. With the analogy to conventional silicon electronics, establishing a method to convert TMDC to p‐ and n‐type semiconductors is essential for various device applications, such as complementary metal‐oxide‐semiconductor (CMOS) circuits and photovoltaics. Here, a successful control of the electrical polarity of monolayer WSe
2 is demonstrated by chemical doping. Two different molecules, 4‐nitrobenzenediazonium tetrafluoroborate and diethylenetriamine, are utilized to convert ambipolar WSe
2 field‐effect transistors (FETs) to p‐ and n‐type, respectively. Moreover, the chemically doped WSe
2 show increased effective carrier mobilities of 82 and 25 cm
2 V
?1s
?1 for holes and electrons, respectively, which are much higher than those of the pristine WSe
2. The doping effects are studied by photoluminescence, Raman, X‐ray photoelectron spectroscopy, and density functional theory. Chemically tuned WSe
2 FETs are integrated into CMOS inverters, exhibiting extremely low power consumption ( ≈ 0.17 nW). Furthermore, a p‐n junction within single WSe
2 grain is realized via spatially controlled chemical doping. The chemical doping method for controlling the transport properties of WSe
2 will contribute to the development of TMDC‐based advanced electronics.
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