TMDCs, [7][8][9] the quantum spin Hall effect, [10] the valleytronics, [11,12] as well as the 2D superconductivity, [13] implying extensive potential applications. In contrast to graphene, monolayer TMDCs with suitable bandgaps have demonstrated the state-of-the-art characteristics for integrated circuits (IC), i.e., high on/ off ratio (>10 7 ) and record drive current density (100 µA µm −1 ). [14,15] So far, a number of approaches have been developed to obtain TMDCs, including the micromechanical cleavage method [16] and liquid-phase exfoliation [17][18][19] due to the weak van der Waals interactions between the neighboring layers. Among them, chemical vapor deposition (CVD) has been widely demonstrated to be an effective technique to synthesize highquality TMDCs as well as their in-plane and vertical heterostructures by using different precursors, [20,21] such as the solid powders of MoO 3 , [22][23][24][25] MoO 3 solution, [26,27] MoCl 5 , [28] WO 3 , [29,30] WS 2 , WSe 2 , MoS 2 , and MoSe 2 [31][32][33] with the additional alkali metal halides as the growth promoters, [2,34] the gaseous chemical precursors including molybdenum hexacarbonyl (MHC), [4] as well as the liquid precursors like the solution of ammonium thiomolybdate (NH 4 ) 2 MoS 4 , [35,36] ammonium molybdate tetrahydrate (NH 4 ) 6 Mo 7 O 24 •4H 2 O and ammonium tungstate hydrate Chemical vapor deposition (CVD) has been widely used to synthesize highquality 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 inkjetprinting 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 MoS 2 and MoSe 2 exhibits excellent electronic properties with carrier mobility up to 21 and 54 cm 2 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.