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The use of volatile solvents for organic synthesis is nowadays questioned due to their negative impact on the environnement. To develop sustainable and environmentally friendly methodologies, we propose to combine two green chemistry concepts: the use of bioinspired solvents: natural deep eutectic solvents (NaDES), and mechanochemistry. Using the Suzuki‐Miyaura coupling as a model reaction, we described an efficient mechanochemical method with NaDES as a LAG (liquid‐assisted grinding) additive with short reaction times and without any ligand or additional heating. A mechanochemical extraction was also used to reduce the amounts of extraction solvents and the total time of the synthesis process. [ABSTRACT FROM AUTHOR]