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The unique structure and properties of two-dimensional (2D) crystals have a large impact on fundamental research as well as applications in electronics,photonics, optoelectronics and energy sciences.Here our recent studies on the controlled synthesis of 2D crystals such as graphene, topological insulator V2VI3 nanostructures, other layered metal chalcogenides and their hybrid materials, as well as their optoelectronic properties will be discussed [1-3].1) We focus on our recent progresses towards the controlled surface growth of graphene and its 2D hybrids via rational designs of chemical vapor deposition (CVD) elementary processes,namely process engineering.