Extraction of active compounds from natural materials is commonly used to produce a diverse range of ingredients, nutrients, drugs, flavors, and fragrances. While solvent-based approaches are standard for these extraction procedures, large solvent volumes, greenhouse gas emission (due to atmospheric release of volatile organic compounds), and large energy requirements are significant issues. Here, we describe a novel process wherein a mechanical action is applied to a solid-state mixture comprising a quaternary ammonium salt and a biological material containing active molecules to form a deep eutectic mixture. It is first shown that eutectic mixtures can be formed for a wide range of naturally occurring compounds. Selective extraction of these compounds from natural products is then demonstrated using rosemary leaves with three different quaternary ammonium salts. The eutectic mixture formed is purified by liquid/liquid extraction using an oily phase to concentrate the active constituents in the deep eutectic phase. The resulting natural extracts are shown to exhibit high antioxidant activities, which were measured using the conjugated autoxidizable triene (CAT) and the oxygen radical absorbance capacity (ORAC) assays.