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Doping can change the intrinsic properties of 2D materials by tuning their electronic structure. In this work, high‐quality 2D In‐doped SnS2 (In‐SnS2) monolayer is reported through chemical vapor transport method and following mechanical cleavage process. The In content of In‐SnS2 is ≈0.9%, and doping results in the downward shift of the Fermi level compared with the undoped one. Transmission electron microscopy images show that doping is uniform in the In‐SnS2 nanosheets with high quality. The In‐SnS2 monolayer field effect transistors (FETs) show p‐type feature which is different from the n‐type feature of undoped SnS2. The average hole produced by one In atom is estimated as 0.37 from FETs measurement. Density functional theory calculations show that the decreasing of hole concentration results from the hole killing mechanism induced by S vacancy. The results suggest that changing the polarity of 2D semiconductor by doping is successful, and In‐SnS2 monolayer has great potential in the applications of electronics and optoelectronics.

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