The layer-by-layer assembly of 2D transition metal dichalcogenide monolayer blocks to form a 3D stack, with a precisely chosen sequence/angle, is the newest development for these materials. In this way, one can create "van der Waals heterostructures (HSs)," opening up a new realm of materials engineering and novel devices with designed functionalities. Herein, a detailed systematic review of transition metal dichalcogenide stacking-engineered heterostructures, from controllable fabrication to typical characterization, and stacking-correlated physical behaviors is presented. Furthermore, recent advances in stacking design, such as stacking sequence, twist angles, and moiré superlattice heterojunctions, are also comprehensively summarized. Finally, the remaining challenges and possible strategies for using stacking engineering to tune the properties of 2D materials are also outlined.

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In article number 2005735, Jiaxu Yan, Wei Huang, and co‐workers systematically review the progress of stacking engineering of transition metal dichalcogenide hetero‐bilayers: from controllable fabrication methods to routine characterization, then to the dependence of interlayer coupling on stacking configurations/angles, and lastly the current challenges and possible future strategies.