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To develop next-generation electronic devices, novel semiconductive materials are urgently required. The transition metal dichalcogenides (TMDs) hold the promise of next generation of semiconductor materials for emerging electronic applications. As a member of the group-10 TMDs, PdS 2 has a notable layer-number-dependent band structure and tremendously high carrier mobility at room temperature. Here, we demonstrate the experimental realization of centimeter-scale synthesis of the few-layer PdS 2 by the combination of physical vapor deposition (PVD) and chemical vapor deposition (CVD) methods. For the first time, the optical anisotropic properties of the few-layer PdS 2 were investigated through angle-resolved polarized Raman spectroscopy. Also, the evolution of Raman spectra was studied depending on the temperature in the range of 12-300 K. To further understand the electronic properties of the few-layer PdS 2 , the field-effect transistor (FET) devices were fabricated and investigated. The electronic measurements of such FET devices reveal that the PdS 2 materials exhibit a tunable ambipolar transport mechanism with field-effect mobility of up to ∼388 cm 2 V -1 s -1 and the on/off ratio of ∼800, which were not reported before in the literature. To well understand the experimental results, the electronic structure of PdS 2 was determined using density functional theory (DFT) calculations. These excellent physical properties are very helpful in developing high-performance opto-electronic applications.