Among transition metal dichalcogenides, molybdenum ditelluride (MoTe2) holds significant attention due to its polymorphic nature including semiconducting, metallic, and topological semimetal phases. Considerable efforts are devoted to synthesizing MoTe2 nanosheets to make them suitable for device integration in nanotechnologies and for fundamental investigations. In this respect, chemical vapor deposition (CVD) via tellurization of a pre‐deposited Mo thin film is an easy and flexible way for synthesizing large scale MoTe2 nanosheets. Here, the study report on the CVD of large‐area (up to 4 cm × 1 cm) MoTe2 nanosheets with pure 1T’ and 2H phase selection by design. Within the tellurization scheme, the vapor‐solid reaction between the pre‐deposited molybdenum film and tellurium vapor is studied thus optimizing the scalability and quality of the MoTe2 nanosheets grown on SiO2/Si substrates. It is …