Thermally evaporated tellurium possesses an intriguing crystallization behavior, where an amorphous to crystalline phase transition happens at near‐ambient temperature. However, a comprehensive understanding and delicate control of the crystallization process for the evaporated Te films is lacking. Here, the kinetics and dynamics of the crystallization of thermally evaporated Te films is visualized and modeled. Low‐temperature processing of highly crystalline tellurium films with large grain size and preferred out‐of‐plane orientation ((100) plane parallel to the surface) is demonstrated by controlling the crystallization process. Tellurium single crystals with a lateral dimension of up to 6 µm are realized on various substrates including glass and plastic. Field‐effect transistors based on 5 °C crystallized Te single grains (6‐nm‐thick) exhibit an average effective hole mobility of ≈100 cm2 V−1 s−1, and on/off current ratio of ≈3 × 104.

Tellurium, as an elemental van der Waals semiconductor, has intriguing anisotropic physical properties owing to its inherent 1D crystal structure. To exploit the anisotropic and thickness‐dependent behavior, it is important to realize orientated growth of ultrathin tellurium. Here, van der Waals epitaxial growth of Te on the surface of 2D transition metal dichalcogenides is systematically investigated. Orientated growth of Te with a thickness down to 5 nm is realized on three‐fold symmetric substrates (WSe2, WS2, MoSe2, and MoS2), where the atomic chains of Te are aligned with the armchair directions of substrates. 1D/2D moiré superlattices are observed for the Te/WSe2 heterostructure. This method is extended to the growth of SeTe alloys, providing flexibility for band engineering. Finally, growth of textured Te film is demonstrated on the lower‐symmetry surface of WTe2.

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