Interest in Metal-Organic Frameworks (MOFs) has been increasing since they were first synthesized in the 1990s. MOFs are a group of nanoporous materials made by combinations of building blocks -metal nodes and organic linkers -assembled into a specific network. The modular nature of MOFs creates an effectively infinite number of possible structures, of which several tens of thousands have been synthesized. MOFs have been synthesized from all corners of the periodic table, giving rise to a wide chemical and physical diversity of MOF structures and properties. The Computation-Ready Experimental (CoRE) database has compiled more than 12000 crystal structures of MOFs and the Cambridge MOF subset currently stands at 88,000 structures, of which ca. 8,000 are porous. While many interesting MOFs and MOF applications have been discovered serendipitously, it is normally desired to design a MOF that possesses some given property. To search for a MOF with some specific property, synthesizing every single MOF is clearly impossible, therefore computational methods have been increasingly employed to guide experiments. One standard procedure is a combinatorial enumeration followed by molecular simulation on every hypothetical structure. Inevitably, the important aspect determining the success of this approach is in the accuracy and efficiency of the molecular simulation methods.