The deep understanding of nucleation and growth mechanisms is fundamental for the precise control of the size, layer number, and crystal quality of two-dimensional (2D) transition-metal dichalcogenides (TMDs) with the chemical vapor deposition (CVD) method. In this work, we present a systematic spectroscopic study of CVD-grown MoS2, and two types of MoS2 flakes have been identified: one type of flake contains a central nanoparticle with the multilayer MoS2 structure, and the other is dominated by triangular flakes with monolayer or bilayer structures. Our results demonstrate that two types of flakes can be tuned by changing the growth temperature and carrier-gas flux, which originates from their different nucleation mechanisms that essentially depends on the concentration of MoO3–x and S vapor precursors: a lower reactant concentration facilitates the 2D planar nucleation that leads to the monolayer/bilayer MoS2 and a higher reactant concentration induces the self-seeding nucleation which easily produces ...