Layered transition-metal dichalcogenides can host multiple crystal structures that are closely spaced in free energy, giving rise to rich electronic diversity under modest external perturbations. Molybdenum ditelluride ($\mathrm{Mo}{\mathrm{Te}}_2$) is a paradigmatic example, in which semiconducting and semimetallic polymorphs closely compete energetically. Here we investigate how hydrostatic compression reshapes electronic transport in bulk $2H\text{−}\mathrm{Mo}{\mathrm{Te}}_2$. At ambient pressure, resistivity and magnetotransport measurements establish a robust insulating ground state governed by strong localization. Upon compression to pressure up to 15.6 GPa, transport evolves continuously from the $2H$ semiconducting regime into an electronic response characterized by large, nonsaturating magnetoresistance and low-temperature quantum-interference effects reminiscent of those reported in semimetallic $1T^{\prime }/\mathrm{Td} \mathrm{Mo}{\mathrm{Te}}_2$. First-principles calculations including spin-orbit coupling reveal a progressive pressure-driven reconstruction of the electronic structure, whereby the indirect band gap narrows and collapses into a semimetallic electronic manifold. Together, these results identify a pressure-tuned localization-to-coherence crossover as the organizing principle of transport in bulk $2H\text{−}\mathrm{Mo}{\mathrm{Te}}_2$, linking disorder-controlled hopping at ambient pressure to quantum-coherent semimetalliclike transport at high pressure. These results demonstrate how lattice compression enables controlled access to competing electronic regimes in layered tellurides and highlight external tuning as a route toward spin-orbit-coupled semimetallic transport states.

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• High magnetic fields
• Magnetoresistance
• Phase transitions
• Pressure effects
• Layered semiconductors
• Transition metal dichalcogenides
• First-principles calculations
• Resistivity measurements