Graphene can be considered as the first two-dimensional covalent polymer prototype. This novel material has caused a deep scientific and even social impact. However, this material lack the rational design and precise control that chemical synthesis can offer. Covalent and metal-organic chemistry allow structural design resulting on materials with predetermined physic-chemical properties unprecedented for organic materials. In this context, the use of covalent organic frameworks (COFs) and metal-organic frameworks could represent a breakthrough Bottom-up and top-down approaches are strategies to be develop with the aim to produce single or few-layers of COFs and MOFs (more..). Our group have been already proof that phase liquid exfoliation of COFs and MOFs is a suitable procedure to generate single/few layers with a reasonable control of the thickness and excellent lateral dimensions. Alternatively, on-surface reactions of selected building blocks show promising results.