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Mate leaves are highly appreciated in south and central America as food ingredient for tea preparation. Their nutritional importance, due to their high content of polyphenols and other nutraceuticals, has been drawing attention worldwide, especially to produce extracts and biopharmaceuticals. However, the extraction of such nutraceuticals using conventional processes/solvents might impact their profile/concentration. Ionic liquids (ILs) and deep eutectic solvents (DES) have been recognized as green solvents, and more recently the naturally-derived have stood out. In this work, we investigated the use of bioethanol, cholinium chloride ([Ch]Cl), Ch-based DES and less expensive protic ILs derived from acetic acid, in aqueous systems at different concentrations, as potential sustainable alternatives over conventional solvents and more expensive aprotic ILs for the extraction of polyphenols from mate leaves. Simply adding the [Ch]Cl in aqueous-ethanolic mixtures at 50% improved extraction efficiency (∼35 mg/g) in comparison to conventional solvents (∼7-29 mg/g). However, IL (∼41-66 mg/g) and DES (∼47-55 mg/g) systems presented better performance, being the former presenting the best results at 75% (∼66 mg/g). The extraction yield was also related to water concentration, which is interesting to reduce viscosity and IL/DES cost for a more cost-efficient extraction and was also supported by results obtained using COSMO-SAC. Therefore, the low-cost protic IL and DES are promising sustainable solvent alternatives over conventional solvents/ILs for extraction of polyphenols from mate leaves., (Copyright © 2022 Elsevier Ltd. All rights reserved.)