The crucial role that defects play in the chemistry of metal-organic frameworks (MOFs) is becoming increasingly clear, with recent studies revealing the existence of defects, especially ligand vacancies, in many important families of MOFs. The presence of defects has been shown to dramatically improve sorption properties [1], catalytic activity [1] and ionic conductivity [2] of MOFs. In many materials, particularly at higher defect concentrations, the interactions between defects lead to nanostructures that determine the behaviour of a material.