The epitaxial growth of low-dimensional tin chalcogenides SnX (X = S, Se) with a controlled crystal phase is of particular interest since it can be utilized to tune optoelectronic properties and exploit potential applications. However, it still remains a great challenge to synthesize SnX nanostructures with the same composition but different crystal phases and morphologies. Herein, we report a phase-controlled growth of SnS nanostructures via physical vapor deposition on mica substrates. The phase transition from α-SnS ( Pbnm ) nanosheets to β-SnS ( Cmcm ) nanowires can be tailored by the reduction of growth temperature and precursor concentration, which originates from a delicate competition between SnS-mica interfacial coupling and phase cohesive energy. The phase transition from the α to β phase not only greatly improves the ambient stability of SnS nanostructures but also leads to the band gap reduction from 1.03 to 0.93 eV, which is responsible for fabricated β-SnS devices with an ultralow dark current of 21 pA at 1 V, an ultrafast response speed of ≤14 μs, and broadband spectra response from the visible to near-infrared range under ambient condition. A maximum detectivity of the β-SnS photodetector arrives at 2.01 × 10 8 Jones, which is about 1 or 2 orders of magnitude larger than that of α-SnS devices. This work provides a new strategy for the phase-controlled growth of SnX nanomaterials for the development of highly stable and high-performance optoelectronic devices.