The phytotoxic residues after olive oil production and residue leaves after pruning contain valuable bioactive compounds. A natural deep eutectic solvent (NADES) and an ethanol-water mixture were used for polyphenol extraction from olive pomace and leaves. Type of solvent, extraction temperature, and particle size of the leaves were optimized. NADES demonstrated better efficiency in the extraction process than conventional solvents; with higher temperature and smaller fraction of olive leaves, a higher yield of polyphenols was obtained from leaves. Extraction with a nanofluid as solvent was carried out. A stable nanofluid was prepared from NADES by adding Al(2)O(3)nanoparticles. A higher yield was obtained with nanofluid from leaves, while an improvement of polyphenol extraction was achieved after the removal of oil from olive pomace.