Tw isted two-dimensional aromatic frameworks have been prepared by overcrowdingthe nodes with bulky and rigid substituents.T he highly distorted aromatic framework with alternating out-of-plane substituents results in diminished interlayer interactions that favor the exfoliation and dispersion of individual layers in organic media.The discovery of graphene [1] has opened up exciting possibilities for developing two-dimensional (2D) polymers, [2] such as 2D conjugated microporous polymers (2D-CMPs) and 2D covalent organic frameworks (2D-COFs), for awide range of applications, [2] including electronics,e nergy conversion and storage,g as storage and separation, catalysis,a nd sensing. Synthetic 2D organic frameworks composed of fused aromatic rings [3] have emerged as ahighly tunable alternative to nanopore-grafted (or holey) graphene,since they combine an extended 2D p system with permanent nanometer-sized pores.F urthermore,s ince such 2D polymers are synthesized by bottom-up approaches,h eteroatoms can be incorporated into the framework with relative ease,w hich provides an additional way to modulate their electronic structure and their properties.F or example,t he exchange of Catoms for Natoms in 2D organic frameworks has resulted in more efficient materials for energy applications,s uch as electrocatalysts for the oxygen reduction reaction (ORR), [4] the hydrogen evolution reaction (HER), [5] supercapacitors, [6] and batteries. [6a, 7] Thepreparation of stable dispersions of individual layers of 2D organic frameworks would be ideal from several perspectives.F irst, it would facilitate the sorting of layers by size,c omposite preparation by solution mixing, chemical modification, and structural and optoelectronic characterization.[8] Second, it would enable the formulation of such 2D materials in inks [8] and thus would enable low-cost, large-area liquid-deposition methods,such as spin coating, spray coating, or inkjet printing.H owever,s imilarly to graphene,s ynthetic 2D organic frameworks are very difficult to process because of the great tendency of the individual layers to aggregate by noncovalent interlayer interactions.A lthough several examples of the delamination of 2D organic frameworks by mechanical [9] and solvent-assisted methods, [10] electrostatic repulsion, [11] and chemical methods [12] have been reported, these methods provide materials that are af ew layers thick and thereby show that the individualization of layers is still achallenging task.Herein, we report anew and unconventional approach for obtaining dispersions of individual layers of 2D-CMPs composed of fused aromatic rings on the basis of the introduction of twists in their framework by overcrowding the nodes of the framework with bulky and rigid substituents, which are forced above and below the plane (Figure 1). The highly distorted aromatic framework with alternating out-ofplane substituents results in diminished interlayer interactions,t hus favoring the exfoliation and dispersion of individual layers in organic ...