In particular, extensive efforts regarding chemical vapor deposition (CVD) methods resulted in a large-scale MoS 2 monolayer of high quality for practical applications. [7][8][9][10][11][12] However, despite the large on-off ratio and high mobility, [3,9] 2D field-effect transistors (FET) composed of monolayer MoS 2 have become burdened with electrical contact issues such as Fermi level pinning (FLP) and high contact resistances. [13][14][15][16][17] The simplest and most abundant mono-sulfur vacancy (V S ) defects in the monolayer MoS 2 cause strong FLP at metal electrodes, which generally induce n-type semiconductor behavior. [18][19][20][21][22] Thus, many methods, which include substitution, charge transfer, intercalation, and electrostatic doping, have been developed to improve the contact properties or modulate the polarity of transition metal dichalcogenides (TMDs). [23][24][25] Meanwhile, the alkali metal halide-assisted CVD methods enable the rapid fabrication of the continuous and waferscale uniform monolayer TMDs directly on several oxide substrates. [26][27][28][29][30][31][32][33][34] Alkali metal cations promote a rapid increase of the single domain size of monolayer TMDs due to dehydration and nucleation suppression, regardless of the halide anions. [28,31,34] However, excess amounts of alkali metals destroy the crystallinity of monolayer TMDs. [29] On the other hand, back-gated FETs based on the MoS 2 monolayers directly grown this way or transferred onto the SiO 2 /Si substrates, used in current Si processing techniques to manufacture electronic devices, [19] showed comparable electrical performances to those fabricated without using alkali metal halides. [8,9,27,34] Nevertheless, such FETs also exhibited n-type behavior. [27,34] Na impurities are notoriously prone to contaminating the SiO 2 surface. [36] Alkali Na metals readily absorb at the oxide substrates during the CVD growth process of monolayer TMDs. [28,29] Furthermore, Na's incorporation at the SiO 2 surface of siloxane or silanol releases electrons into the monolayer MoS 2 conduction band; [37] whereas, in graphene deposited on SiO 2 , Na produces holes. [38] To understand the effect of trapped Na cations, we synthesized the large-scale uniform MoS 2 monolayers on the SiO 2 / Si substrates using NaCl catalysts [27] and then performed two-probe I-V measurements by the forward and reverse bias sweeping between ±30 V in the ambient air condition at room temperature (see Figures S1-S3, Supporting Information). Notably, initial low or negligible source/drain I-V signals in the µA range enhanced to the mA range after the Alkali metal halide-assisted chemical vapor deposition (CVD) methods can produce wafer-scale uniform monolayer transition metal dichalcogenides (TMDs). Further defect engineering is necessary to obtain high-performance functional devices. While defect engineering has focused on the surface of the monolayer TMDs or the contact property, interface defect engineering is rare and non-trivial. Based on a NaCl-assisted CVD-grown l...