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The SiS 2 rods exhibit a significant anisotropy property applied in a special field such as in the one of all-solid-state lithium-ion batteries and so on. In this work, the orthorhombic SiS 2 rods with high chemical/phase purity were prepared by an elemental method, either through a boiling or a steaming process, at 1023–1073 K for 3 h and under the saturated S-vapor pressure (2.57–3.83 MPa) in a closed sealed-tube system. The composition, crystal structure, morphology, and growth mechanism were investigated. Results showed that the growth orientation of SiS 2 along the <0 0 1> is intrinsically governed by the crystal structure motif. It could exist in both processes and the latter tends to show in macroscopic morphology. Using the pressure-temperature diagram, structure refinement, pole figures, image analyses, and so forth, factors influencing the purity and growth of SiS 2 rods were concluded from the thermodynamics and kinetics viewpoints.