Magnetic field-tunable transport phenomena, especially giant magnetoresistance in quantum materials, remain critical for unlocking fundamental physics and next-generation spintronic devices. Here, we synthesized a series of $\mathrm{ZrT}{\mathrm{e}}_5$ single crystals with different Te deficiencies through precisely controlling growth conditions. By systematically tuning Te-vacancy concentrations in $\mathrm{ZrT}{\mathrm{e}}_5$ crystals, we observe a progressive suppression of the resistivity cusp from 135 to 2 K, where the near-stoichiometric one exhibits semiconducting behavior. Magnetoresistance of the as-synthesized ${\mathrm{ZrTe}}_5$ single crystals can also be manipulated, reaching a maximum of $1.12\times {10}^4\%$ at 2 K and 9 T. A Two-band model analysis of magnetoresistance and Hall resistance reveals that the unique transport evolution originates from defect-induced variations in Fermi level, which affect the carrier concentration and mobility within $\mathrm{ZrT}{\mathrm{e}}_5$ crystals. Our work proposes that engineered defects may open up an avenue to tailor the physical properties of $\mathrm{ZrT}{\mathrm{e}}_5$ and related materials and explore different device functionalities.

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• Crystal defects
• Hall effect
• Magnetotransport
• Single crystal materials
• Topological materials
• Crystal growth
• Energy-dispersive x-ray spectroscopy
• Methods in transport
• Raman spectroscopy
• Transport techniques