LAUSR

2D transition metal dichalcogenides (TMDs) have emerged as an ideal alternative to silicon in advanced electronics. Especially, MoTe2 attracts peculiar attention since it offers a unique opportunity of resolving critical electrical contacts. Currently, although MoTe2‐based coplanar semiconductor‐metal circuitry realized by epitaxial growth and chemical assembly has been demonstrated, while still suffers from the requirement of extremely accurate synthesis process control. Here, a facile strategy is demonstrated to fabricate large scale and high performance MoTe2 transistors with a 1T'/2H vertical homojunction structure by combining a spatial and phase controlled MoTe2 scalable synthesis and a scalable universal transfer method with water‐soluble poly‐vinylpyrrolidone and poly‐(vinyl alcohol) bilayer mediator. Both high quality 1T'‐ and 2H‐ MoTe2 with controlled dimensions can be scalable synthesized via a shadow mask assisted chemical vapor deposition method. These as‐synthesized MoTe2 patterns can be successfully transferred to a wide range of substrates at a high yield >80% with well‐retained properties to construct transistors with a complex vertical 1T'/2H‐MoTe2/HfAlO2 structure. The devices exhibit an on/off current ratio surpassing 104 and a typical mobility of ≈29 cm2 V−1 s−1. The developed scaled strategy of combining both scalable MoTe2 synthesis and transfer offers a feasible way for potential MoTe2‐based large‐scale electronics.