field-effect transistors (FETs) as promising candidate to replace or supplement the current silicon-based technologies in scaled integrated circuit. [4,5] Nevertheless and regrettably, other possible applicability such as TMDs-based thin film transistors (TFTs), which feature the vital applications like large-area and flexible electronics, was rarely systematically demonstrated. [6] Differing from high-performance TMDs FETs as possible alternative to silicon, low cost and simplicity of fabrication process are especially critical for applications of TMDs-based TFTs, except for their basic requirement of device performance. [1] In this regard, the technology of high-k dielectric film fabrication attracts particular concern as the key step of the TFTs fabrication process. Currently, although vacuum-based dielectric film technology such as physical vapor deposition, chemical vapor deposition (CVD), and atomic layer deposition (ALD) was commonly used for high performance TMDs FETs, these technologies still suffer from the inevitable disadvantages such as high cost, time-consuming, and relying on high vacuum environment. [8][9][10] Conversely, solution-processed high-k dielectrics are highly preferable and might be the most suitable approach for TMDs-based TFTs due to its characteristics of low cost, simple process, high throughput, and especially high composition controllability to fabricate ternary oxide dielectrics by adjusting precursor solutions, which is capable of effectively improving device performance by combining the advantages of different binary oxide dielectrics. [11][12][13] Therefore, systematic investigation of TMDs-based TFTs with solutionprocessed ternary high-k dielectrics is desirable and fundamentally essential for their diverse applications.Herein, following our previous scalable synthesis and transfer of (MoTe 2 ) patterns, [14,15] we further report high-performance and low-power CVD-grown polycrystalline MoTe 2 TFTs with solution-processed ternary Hf 0.5 Zr 0.5 O 2 /HfAlO 2 high-k dielectrics. Among TMDs family, MoTe 2 is especially appealing for TFTs application since wafer-scale phase-controlled synthesis can be readily achieved, [16] which benefits for both easy device fabrication and homojunction-based electrical contact improvement. [15,[17][18][19][20] In this manuscript, first, we focus Besides the widely investigated potential as alternative to silicon in microelectronics, semiconducting 2D transition metal dichalcogenides (TMDs) also show appealing prospects in thin film transistors (TFTs)-based applications, while still suffer from insufficient demonstration. Herein, the authors systematically report high-performance and low-power chemical vapor deposition-grown polycrystalline molybdenum ditelluride (MoTe 2 ) TFTs with solution-processed ternary Hf 0.5 Zr 0.5 O 2 /HfAlO 2 high-k dielectric. Benefitting from the optimized high quality HfAlO 2 film synthesis and proper postannealing treatment, the constructed MoTe 2 TFTs exhibit a high mobility ≈27.24 cm 2 V −1 S −1 , a current on/off ...