Two-dimensional crystals are a class of materials in which an individual layer is indefinitely extended in two dimensions. Each layer is the molecular unit in the crystalline lattice. The nature of interlayer/intermolecular interaction is poorly understood. However, it defines physical properties such as carrier mobility, thermal conductivity, photoluminescence, etc. The vibrational properties of 2D materials are described based on triperiodic space groups. However, the triperiodic space groups do not apply to the description of these structures. The 17 two-dimensional groups in triperiodic space groups do not allow the existence of a third dimension. Therefore, if structures are not planar, the approach is inappropriate. The way to describe such structures is using the diperiodic groups in three dimensions. The well-known 2D materials are graphite, graphene, chalcogenide of Ga, Mo, W, and other elements. The crystalline As2S3 belongs to a class of 2D materials. The unit cell contains two layers with ten atoms in each layer, and it is similar to a structure of metal chalcogenide (MoS(Se)2, WS(Se)2). A bond length of 2.24 A is within the layer, and 3.56 A is between the layers. This interlayer/intralayer bond length ratio (= 1.59) corresponds to a significant difference in bond strengths. Center-zone optical phonons in crystalline As2S3 have been investigated by Raman scattering in a wide temperature range for two polarizations in the layer plane (ac). The crystal's and individual layers' symmetry are different, defining different selection rules for optical phonons. According to the crystallographic data, crystal symmetry is monoclinic with 20 atoms in a unit cell and is P21/n (C2h 5). The axis b, perpendicular to the layers, is the only unique axis of the crystal. Therefore, all phonons in the ac plane should be indistinguishable. The layer symmetry is orthorhombic in the diperiodic space group in three dimensions, in which a, b, and c axes are axes of symmetry with a space group of Pnm21 (C2v 7). The intensity of Raman bands in the layer plane shows strong polarization dependence, indicating layer symmetry's dominance. Interlayer interaction is weak, and as a result, low-frequency Raman bands appear in the spectra. The position of these bands defines the strength of interlayer interaction. The data presented provides an understanding of the structural motives of 2D As2S3 and may predict the optical/electronic properties of similar 2D materials based on Raman spectra.