1 of 6) 1600814and optical absorption behaviors of GeS nanosheets have been studied and proposed for energy applications, [16,17] however, the light-emitting property of a thin multilayer GeS was not yet explored.Herein, in-plane optical anisotropy of band-edge emission of a multilayer GeS stripe (t ≈ 40 nm) is characterized by using polarized micro-photoluminescence (µPL) measurement with polarization angles ranging from 0 to 90° with respect to the multilayer's longest crystal edge (b axis). Light emission from multilayer GeS is completely forbidden at θ = 0° (E||b), and fully allowed (intense light) at θ = 90° (E||a), which obeys a dichroic Malus law [18] for the emission peak at 1.622 eV. Multilayer GeS behaves like a dichroic light emitter with linear polarization along the multilayer's a axis. To understand the band-edge characteristic of the GeS multilayer, polarized thermoreflectance (PTR) measurement by using microscope white-light guiding was also implemented. The selection rule of the PTR spectra also reveals that the lower band-edge transition E A = 1.622 eV is only allowed with E||a polarization while another higher energy transition, E B = 1.732 eV, appears merely along the E||b polarization in the multilayer. In-plane anisotropy of the c plane GeS multilayer occurs with linear polarization along a and b axes. The energy position of the E A transition matches well with the main band-edge emission observed by µPL, while the E B transition may probably originate from valence-band splitting (dominated by the S p orbital) of the multilayer GeS. The structural and optical anisotropy of the multilayer GeS is discussed here.Layered single crystals of IV-VI GeS with different areas, sizes, and thicknesses were grown by using the chemical vapor transport (CVT) method [19] with iodine as the transport agent. The crystals were prepared from their elements (Ge: 99.999% pure and S: 99.999%) by reaction at 600 °C for two days in evacuated quartz ampoules. Sulfur was added in 1 mol% excess with respect to the stoichiometric mixture of the constituent elements. About 10 g of the elements, together with an appropriate amount of transport agent (I 2 about 10 mg cm −3 ), were introduced into a quartz ampoule (22 mm OD, 17 mm ID, 20 cm length), which was then cooled with liquid nitrogen, evacuated to 10 −6 Torr and sealed. The mixture was slowly heated to 600 °C and maintained at this temperature for two days. The temperature was then altered from 600 °C (heating zone) → 520 °C (growth zone) with a gradient of -4 °C cm −1 for crystal growth. The reaction was left 240 h to produce large single crystals. The as-grown GeS crystals are dark red and have a shiny surface with an area of up to 5 mm 2 and thickness of up to 100 µm. The crystals are mostly like ribbon or stripe-shape layered crystals (see Figure S1 in the Supporting Information). The powder and single-crystal X-ray diffraction (XRD) results of GeS shown in Figure S1 reveal an orthorhombic phase. The lattice constants are a = 4.36 Å, b = 3.67 Å, and c = 10.53 Å,