The development of simple, versatile strategies for the synthesis of gold nanoparticles (AuNPs) on semiconducting transition metal dichalcogenides (TMDC) layers is of increasing scientific and technological interest in photocatalysis, optical sensing, and optoelectronics sectors, but challenges exist on the nucleation and hybridization of AuNPs with the TMDC basal plane. At present, the widely used aqueous solution approaches suffer from poor dispersion of produced hybrids as well as from limited growth and coverage of the AuNPs on the TMDC semiconducting plane, since Au nanoclusters nucleate preferentially at the electron rich defect edges, which act as reducing agents and not on the defect free basal plane. Here, we report for the first time, the controlled synthesis of AuNPs on the basal plane of semiconducting molybdenum disulfide nanosheets (2H-MoS2 NSs) via a N,N-dimethylformamide (DMF)-based hot-injection synthesis route. This organic solvent-based synthesis route eliminates problems of poor dispersion of AuNPs@2H-MoS2 NS hybrids, whereas at the same time maintains the semiconducting crystalline quality of the pristine 2H-MoS2 NSs. In addition, the study establishes the important role of trisodium citrate, on enhancing the nucleation and improving the hybridization of AuNPs on 2H-MoS2 NSs as evidenced by the induced p-type doping. This organic solvent synthesis approach can be adopted for other hybrid systems opening the way for controlled hybridization of semiconducting layers with metal nanoparticles. 4 MoS2 NSs of metallic phase (M-MoS2), produced by Li intercalation, where dominance of defects on the basal plane promoted the MoS2/ + redox reaction. 2-3 Nevertheless, many applications such as photocatalysis, optical sensing, and optoelectronics, favor the presence of a semiconducting-TMDC/metallic-NP interface to increase absorption, enhance photogeneration rate and/or achieve light induced charge separation. 15 As a result, the growth of AuNPs on semiconducting 2H-MoS2 is been sought. However, whereas the anchoring of AuNPs on M-MoS2 has been explored thoroughly, 2-3 strategies for synthesis of AuNPs on semiconducting 2H phase TMDCs (2H-TMDC), (AuNPs@2H-TMDC), are currently at incipient stages. 10, 16 To tackle this challenge, routes for producing solvent-dispersible hybrids, with a controlled nucleation and coverage of AuNPs on the 2H-TMDC basal plane are being avidly sought.Recently, the functionalization of 2H-TMDC, using chemical reactions of gold precursors in aqueous solution, has been explored. 16 However, the Au-nucleation was limited mainly at the electron rich edges, 16 due to the absence of highly energetic defects on the basal plane, whereas the efficient synthesis of hybrids was hindered by the poor dispersion of semiconducting 2H-MoS2 NSs in water. Lately, we reported the production of 2H-MoS2 NSs, via room temperature ionic liquid (RTIL) assisted grinding method combined with sequential centrifugation steps. 17 Such mechanically exfoliated 2H-MoS2 NSs retain their crystalline quality aft...