Two-dimensional metallic NbS 2 has attracted increasing attentions due to its excellent properties. So far, the preparations of NbS 2 are mainly focused on the mechanical exfoliation and molecular beam epitaxial (MBE), both of which have limitations, such as, small lateral sizes (usually <1 µm), low yield, etc. Chemical vapor deposition (CVD) has been used to synthesize NbS 2 , but mainly depends on atomically flat substrates (e.g., graphene, h-BN) to grow thinner and larger sheets and the growth of NbS 2 on SiO 2 /Si is still challenging. In this contribution, NbS 2 single crystals with different layers are controllably synthesized. Few-layer NbS 2 single crystals from one layer to nine layers with several tens of micrometers lateral sizes (up to ∼20 µm) can be obtained by controlling hydrogen content in Ar/H 2 carrier gas, NaCl amount, the growth temperature and the growth time, which are much larger than that synthesized by the MBE route. Meanwhile, as-synthesized NbS 2 demonstrates higher sensitivity for probing trace amount of molecules than that of graphene, ascribed to the efficient charge transfer between NbS 2 and molecules.