The chiral helimagnetic material Cr_1/3TaS₂ features strong spin-lattice coupling effects and unique topological magnetic states, making it an ideal platform for exploring spintronics and quantum transport phenomena. In this study, high-quality Cr_1/3TaS₂ single crystals were synthesized via the chemical vapor transport method. We systematically investigated the in-plane electrical transport and magnetoresistance evolution of the material over a broad pressure range of 0.6 to 34.0 GPa. High-pressure measurements were conducted using a diamond anvil cell with a standard four-probe configuration in a physical property measurement system, covering temperatures down to 2 K and magnetic fields up to 9 T. Our experimental results reveal a complex, pressure-induced evolution of the electronic and magnetic ground states. In the low-pressure regime (0.6-5.0 GPa), the material maintains robust metallicity, while the long-range magnetic ordering transition temperature TC is significantly suppressed from ~150 K down to ~75 K, driven by enhanced interlayer coupling and modulated Ruderman-Kittel-Kasuya-Yosida interactions. As pressure increases to the intermediate range (7.0-20.0 GPa), the system exhibits an anomalous semiconductor-like transport behavior. However, the absolute resistivity remains on the order of a moderate conductor, suggesting that the scattering mechanism is dominated by weak localization effects or the opening of a pseudogap at the Fermi surface rather than a complete metal-insulator transition. Upon further compression above 23.0 GPa, extreme volume reduction induces severe band broadening, which overcomes the localization potentials and drives a re-entrant transition back to a conventional metallic state. Crucially, magnetoresistance measurements reveal a distinct sign reversal from negative to positive at 13.0 GPa. This anomaly provides compelling evidence for a pressure-induced "spin collapse" effect, marking the dissolution of the long-range magnetic ordered state and the severe suppression of local magnetic moments. This work elucidates the pressure-dependent electronic landscape of Cr_1/3TaS₂, providing vital experimental insights into the intricate interplay among the lattice, charge, and spin degrees of freedom in intercalated van der Waals magnetic materials.