Magnetron-sputtered MoS2 has applications in piezoresistive functional materials research owing to its unique nanostructure. However, the controlled incorporation of sulfur vacancies and realization of enhanced piezoresistive performance remain significant challenges. In this work, the direct growth of large-area MoS2 films with tunable sulfur vacancy concentrations was successfully achieved via magnetron sputtering at various temperatures. Microstructural analysis revealed that the application of strain altered the number of conductive channels between the vertical MoS2 nanosheets, changing the measured resistance and leading to excellent piezoresistive properties. More importantly, the unsaturated electrons due to the sulfur vacancies increased the in-plane carrier concentration of the MoS2 nanosheets. A deposition temperature of 50 °C afforded the highest concentrations of sulfur vacancies and carriers. These MoS2 films possessed a carrier concentration of 6.58 × 1017 cm−3, which was 40.9% higher than that obtained at 150 °C, and displayed superior piezoresistive performance. The films exhibited high gage factors of 2.66 and 23.22 under tensile and compressive strain of ≤0.29%, respectively. These values were 118% and 323% higher, respectively, than those obtained for films deposited at 150 °C. This work provides an effective route for modulating and mass producing MoS2-based piezoresistive electronic devices.