Abstract2D van der Waals (vdW) heterostructures are receiving increasing research attention due to the theoretically amazing properties and unprecedented application potential. However, the as‐synthesized heterostructures are generally underperforming due to the weak interlayer coupling, which inspires the researchers to find ways to modulate the interlayer coupling and properties, realizing the tailored performance for actual applications. There have been a lot of publications regarding the controllable regulation of the structures and properties of 2D vdW heterostructures in the past few years, while a review work summarizing the current advances is not yet available, though it is significant. This paper conducts a state‐of‐the‐art review regarding the current research progress of performance modulation of vdW heterostructures by different techniques. First, the general synthesis methods of vdW heterostructures are summarized. Then, different performance modulation techniques, that is, mechanical‐based, external fields‐assisted, and particle beam irradiation‐based methods, are discussed and compared in detail. Some of the newly proposed concepts are described. Thereafter, applications of vdW heterostructures with tailored properties are reviewed for the application prospects of the topic around this area. Moreover, the future research challenges and prospects are discussed, aiming at triggering more research interest and device applications around this topic.

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