offers advantages over simple inorganic nanosheets in that a diverse range of physical and chemical properties can be programmed into their crystalline structure (Figure 1). This distinct combination of properties makes MONs ideal for a wide range of catalysis, sensing, electronics, and separation applications which will be the focus of this review.Much of the early literature in this field focused on the development of novel MON architectures and new routes towards their synthesis. A diverse range of different metal ions and organic linkers have been used to construct MONs. [4] However the field has rapidly converged on a handful of popular secondary building units (SBUs) which dominate much of the literature thanks to their reliable formation of high aspect ratio nanosheets. Popular classes of MONs that have been widely applied by different groups in applications include those based on the metal paddlewheel (PW) motif, [5][6][7] axially capped Zr and Hf clusters, [8][9][10][11] 2D zeolitic imidazolate frameworks (ZIFs), [12][13][14] and square planar Ni, Co, and Cu SBUs. [15][16][17][18] The modular structure of MONs, ease of functionalization and diverse range of materials they can be combined with means that MONs can be readily "programmed" to provide the desired topology and properties required for a given application.A wide variety of methods have been explored to synthesize MONs, either "top-down" by the exfoliation of layered metalorganic frameworks (MOFs) or "bottom-up" by assembly of molecular building blocks directly into nanosheets. The majority of top-down approaches utilize mechanical energy to overcome inter-layer interactions, such as liquid-assisted ultrasonication, [19] shear-mixing, [20] and grinding/ball-milling, [13] or the less common freeze-thaw [21] and "scotch-tape" methods. [22,23] Other methods involving photochemical, [24] electrochemical, [25] and chemical intercalation, [26] have also been developed but are less widely used. Bottom-up methodologies typically utilize surfactants or modulators to inhibit crystal growth in one dimension, [12,27,28] or layering/interfacial methods to promote anisotropic growth. [15,29,30] The use of sacrificial 2D templates has also recently emerged a promising route. [31,32] Each approach has advantages and disadvantages in terms of the thickness, lateral dimensions, size distribution, quantity and quality of the MONs produced, and the best approach therefore varies depending on the application.