The combination of two-dimensional (2D) materials with non-2D materials (quantum dots, nanowires and bulk materials), i.e. mixed-dimensional van der Waals (md-vdW) heterostructures endow 2D materials with remarkable electronics properties. However, it remains a big challenge to synthesize md-vdW heterostructures because of the difference of crystal symmetry between 2D and non-2D materials. Meanwhile, it is difficult to initiate the nucleation due to the lack of chemical active sites on chemical inert surfaces of 2D materials. Herein, we design a general chemical vapor deposition method for synthesizing a broad class of md-vdW heterostructures with well-aligned hexagonal symmetry including MoS₂/FeS, MoS₂/CoS, MoS₂/MnS, MoS₂/ZnS, Mo(S _x Se_1–x )₂/ZnS _x Se_1–x , Mo(S _x Se_1–x )₂/CdS _x Se_1–x . Combining with DFT calculation, we find that the hexagonal symmetry and the centered clusters of MoS₂ and Mo(S _x Se_1–x )₂ nanoflakes are two crucial factors to launch the hexagonally oriented growth and nucleation of non-2D materials on 2D materials. Our discovery opens an opportunity for the versatile hetero-integration of 2D materials and allows systematic investigation of physical properties in a wide variety of md-vdW heterostructures.

二维 (2D) 材料与非二维材料（量子点、纳米线和块状材料）的组合，即混合维范德华 (md-vdW) 异质结构赋予二维材料卓越的电子特性。然而，由于二维和非二维材料之间晶体对称性的差异，合成 md-vdW 异质结构仍然是一个很大的挑战。同时，由于二维材料的化学惰性表面缺乏化学活性位点，难以引发成核。在此，我们设计了一种通用的化学气相沉积方法，用于合成广泛的具有对齐六边形对称性的 md-vdW 异质结构，包括 MoS ₂ /FeS、MoS ₂ /CoS、MoS ₂ /MnS、MoS ₂ /ZnS、Mo(S _x Se _{1– x} ) ₂ /ZnS _x Se _{1– x} , Mo(S _x Se _{1– x} ) ₂ /CdS _x Se _{1– x}。结合DFT计算，我们发现MoS ₂和Mo(S _x Se _{1– x} ) ₂的六边形对称性和中心簇 纳米薄片是在二维材料上启动非二维材料的六边形取向生长和成核的两个关键因素。我们的发现为二维材料的多功能异质集成提供了机会，并允许系统研究各种 md-vdW 异质结构的物理特性。