Rare-earth tri-iodides (RI₃) are a series of two-dimensional van der Waals (vdW) magnetic materials comprising a layered honeycomb structure. Both the growing interest in vdW magnetic systems and the honeycomb layered structure of RI₃ compounds, which is essential for realizing Kitaev physics, motivated us to grow high-quality single crystals of this series of materials and investigate their ground-state magnetic properties. Here, we report the crystal growth, magnetic, and thermodynamic properties of large (centimeter-sized), high-quality crystals of RI₃ compounds. The crystal growth uses the physical vapor transport method via self-transport reaction using iodine as a transporting agent. The growth parameters are meticulously reported. The crystallographic parameters are obtained using single-crystal x-ray diffraction. While the RI₃ compounds for the lighter rare earths (R = La and Ce) crystallize with an orthorhombic (Cmcm) structure, the structure for the heavier rare earths is trigonal (R3̄), analogous to the extensively investigated Kitaev material α-RuCl₃. The density functional theory–based calculations are performed to obtain the eigenfrequencies/eigenvectors of the Raman-active phonon modes for both structure types and compared with the experimental Raman spectra of CeI₃ (Cmcm) and HoI₃ (R3̄). The magnetic behavior examined for the heavier rare-earth-based compounds indicates no signs of long-range magnetic ordering down to 2 K. However, signatures of short-range correlations are seen below 5 K, both in the magnetic susceptibility and specific heat of all the compounds.