The structural dynamics of Thallium Indium Disulfide (TlInS2) crystal under elevated pressures were comprehensively investigated using a combination of X-ray diffraction (XRD), Raman spectroscopy via first-principles calculations, and Hirshfeld surface (HS) analysis. This study aims to elucidate pressure-induced modifications in the crystal structure and their associated properties of TlInS2 crystal. The findings reveal significant structural transformations as pressure increases, with XRD patterns indicating lattice compression and a critical transition from semiconductor to conductor at pressure P=6.25GPa [42]. The calculations predict a reduction in bond lengths, specifically S1-In1 and S1-Tl2, alongside a corresponding decrease in lattice parameters and unit cell volume. Raman spectroscopy corroborates these changes through shifts in phonon modes. The HS analysis provides further insights into pressure-dependent alterations in intermolecular interactions, revealing changes in voids and surface characteristics. The data gained from TlInS2's structural behavior under pressure, contributing to the optimization of its functional properties for pressure-tunable applications in high-performance electronic and optoelectronic devices.