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Li/MgO is one of the most frequently investigated catalysts for the oxidative coupling of methane. Besides catalytic testing, it is also a suitable system to perform surface science experiments and quantum chemical calculations, which is not possible for many other active catalysts. However, the real structure of Li/MgO, the nature of the active center and the structure - activity relationship remain unclear, despite all the research that has been done. The aim of this review is to summarize the available knowledge on Li/MgO to structure and accelerate and improve the ongoing work on this catalytic system.