Two-dimensional transition metal dichalcogenide (TMDC) nanocrystals (NCs) exhibit unique optical and electrocatalytic properties. However, the growth of uniform and high-quality NCs of monolayer TMDC remains a challenge. Until now, most of them are synthesized via a solution-based hydrothermal process or ultrasonic exfoliation method, in which the capping ligands introduced from organic solution often quench the optical and electrocatalytic properties of TMDC NCs. Moreover, it is difficult to homogeneously disperse the solution-based TMDC NCs on a substrate for device fabrication, since the dispersed NCs can easily aggregate. Here, we put forward a novel CVD method to grow closely spaced MoS2 NCs around 5 nm in lateral size. TEM and AFM characterizations demonstrate the monolayer and high-crystalline nature of MoS2 NCs. An obvious blue-shift with 130 meV in photoluminescence signals can be observed. The MoS2 NCs also show an outstanding surface-enhanced Raman scattering for organic molecules due to their localized surface plasmon and abundant edge sites and exhibit excellent electrocatalytic properties for the hydrogen-evolution reaction with a very low onset potential of ∼50 mV and Tafel slope of ∼57 mV/decade. Finally, we further demonstrate this kind of CVD method as a versatile platform for the growth of other TMDC NCs, such as WSe2 and MoSe2 NCs.