“…Among all, recently discovered 2D covalent organic frameworks (COFs) have attracted great attention because of their tailorable structures and affordable functionalizations at the molecular level. − These materials designed via the reticular approach (utilizing kinetically reversible reactions) result in layered structures of highly conjugated nanosheets which are held together through intermolecular forces such as π–π interactions or, in some cases, hydrogen bonding. , These forces play a crucial role in producing highly crystalline, stable COFs with 1D nanochannels for various applications. − However, some adverse effects of these layered structures such as aggregation-caused quenching (ACQ), poor electron mobility, and poor accessibility of deeply buried active sites in the nanochannels lead to the moderate performance of 2D COFs, especially for applications where photoluminescence properties and fast response–recovery are concerned . To counter these negative effects, exfoliation of COFs has been explored via mechanical delamination, chemical modification, , and ultrasonification , to produce the nanosheets of a single layer or a few layers. − However, these techniques also have some disadvantages such as small-scale processing, alteration of the original chemical structure, high energy consumption, and so forth, which limit their widespread use in large scale commercial applications. These issues, however, can be addressed via developing self-exfoliable 2D COFs − to produce smart materials with tuneable photoluminescence properties and well-exposed active sites for desired applications.…”