Atomic‐Scale Structural Modification of 2D Materials

2D materials have attracted much attention since the discovery of graphene in 2004. Due to their unique electrical, optical, and magnetic properties, they have potential for various applications such as electronics and optoelectronics. Owing to thermal motion and lattice growth kinetics, different atomic‐scale structures (ASSs) can originate from natural or intentional regulation of 2D material atomic configurations. The transformations of ASSs can result in the variation of the charge density, electronic density of state and lattice symmetry so that the property tuning of 2D materials can be achieved and the functional devices can be constructed. Here, several kinds of ASSs of 2D materials are introduced, including grain boundaries, atomic defects, edge structures, and stacking arrangements. The design strategies of these structures are also summarized, especially for atomic defects and edge structures. Moreover, toward multifunctional integration of applications, the modulation of electrical, optical, and magnetic properties based on atomic‐scale structural modification are presented. Finally, challenges and outlooks are featured in the aspects of controllable structure design and accurate property tuning for 2D materials with ASSs. This work may promote research on the atomic‐scale structural modification of 2D materials toward functional applications.