Two-dimensional layered MoS₂ nanosheets exhibit a wide range of attractive properties and hold great promise in myriad fields. However, the poor performance of surface functionality greatly limits their applications. In this paper, we report on a facile approach to direct synthesis of organic functional group decorated MoS₂ (OFGD-MoS₂) nanosheets based on the simultaneous exfoliation of bulk MoS₂ crystals and chemical conjugation of thiol ligands. The morphology and structure of OFGD-MoS₂ nanosheets are systematically characterized using microscopy (TEM, SEM, AFM), thermal gravimetric analysis (TGA), and spectroscopy (Raman, FTIR, XPS) measurements. The content of attached functional groups can be controlled simply by changing the experimental conditions. Furthermore, the introduced functional groups show excellent structural stability and high chemical reactivity, making them promising for further modification as confirmed by the in situ growth of inorganic nanoparticles and polymers. In addition, surface functionalized WS₂ nanosheets can also be synthesized by this approach. This investigation paves the way for the synthesis and applications of advanced MoS₂-based materials.