www.advmat.de www.advancedsciencenews.com production challenging. Since the discovery of the chemical vapor deposition (CVD) method as a successful approach for the growth of graphene crystals, [53,54] the method has also been expanded to the preparation of other 2D layered materials. Currently, this approach has been extended to rationally design various 2D TMD materials, such as MoS 2 nanosheets, [55][56][57][58] MoSe 2 nanosheets, [59,60] WS 2 nanosheets, [61,62] ReS 2 nanosheets, [63] and some heterostructures, [64,65] which have sparkled several interesting chemical and electronic properties. Although various 2D TMDs have been successfully grown using a facile CVD method, the intrinsic growth mechanism and the batch production of wafer-scale films, conducive to the high-performance in electronics/optoelectronics and other fields, still need more exploration. Very recently, some important progress on the synthesis of 2D TMDs, multi-heterostructures and superlattices has been realized.Herein, we concentrate on the recent progress in the synthesis of 2D TMDs and related heterostructures via the CVD method. We start with the effects of some key factors such as temperature, carrier gas, and the ratio of precursors on the synthesis of 2D TMDs via CVD technique. Then we summarize the importance of the growth substrates and the growth system to large-scale synthesis. Hence, large-scale 2D TMDs have been obtained on the basis of properly designed CVD growth. Furthermore, some recent breakthroughs in the growth of new kinds of semiconducting and metallic 2D TMDs via the CVD technique are described. The fundamental electronic properties and unique physical phenomena emanating from high quality CVD-grown TMDs are also reviewed. Finally, the controlled growth of alloys with tunable band structures, different multiheterostructures with atomically sharp interfaces and superlattices from 2D TMD crystals is analyzed, which can offer further step for the synthesis of 2D crystals and provides significantly more material systems. Lastly, we emphasize a summary of this review and the future prospects of these materials.Recently, the CVD method has been widely regarded as a technique available for growing 2D atomic crystals. Various atomically thin layered MX 2 semiconductors, such as MoS 2 , [55,66,67] WS 2 , [68] MoSe 2 , [69] MoTe 2 , [70,71] etc., have been successfully achieved by the CVD method. Through in-depth research on the growth dynamics in the CVD system, several key factors in the growth process for obtaining a large-scale, uniform monolayer MX 2 have been explored. For example, triangular WS 2 flakes were synthesized on a sapphire substrate via a CVD system, and a detailed analysis of the controllable growth behavior was given. [61] The growth system is maintained at a very low pressure during the growth process via an operating pump, which provides a uniform flow of vapor precursors and is beneficial to the uniform growth. First, the distance between the source and substrate (D ss ) was discovered to be a vital fa...