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Chemical vapor deposition (CVD) has been widely used to synthesize high‐quality 2D transition‐metal dichalcogenides (TMDCs) from different precursors. At present, quantitative control of the precursor with high precision and good repeatability is still challenging. Moreover, the process to synthesize TMDCs with designed patterns is complicated. Here, by using an industrial inkjet‐printer, an in situ aqueous precursor with robust usage control at the picogram (10−12 g) level is achieved, and by precisely tuning the inkjet‐printing parameters, followed by a rapid heating process, large‐area patterned TMDC films with centimeter size and good thickness controllability, as well as heterostructures of the TMDCs, are achieved facilely, and high‐quality single‐domain monolayer TMDCs with millimeter‐size can be easily synthesized within 30 s (corresponding to a growth rate up to 36.4 µm s−1). The resulting monolayer MoS2 and MoSe2 exhibits excellent electronic properties with carrier mobility up to 21 and 54 cm2 V−1 s−1, respectively. The study paves a simple and robust way for the in situ ultrafast and patterned growth of high‐quality TMDCs and heterostructures with promising industrialization prospects. Moreover, this ultrafast and green method can be easily used for synthesis of other 2D materials with slight modification.
Large‐area patterned transition‐metal dichalcogenide (TMDC) films with centimeter size and good controllability of the thickness and TMDC heterostructures are achieved by a facile, low‐cost strategy involving printing using an industrial inkjet‐printer with precisely tuned inkjet‐printing parameters followed by a rapid heating process. High‐quality single‐domain monolayer TMDCs with millimeter size can be easily synthesized within 30 s by this method.