Extracts rich in antioxidants, such as rosemary extracts, are currently obtained by extraction of the plant material using hydro-alcoholic mixtures with high ethanol content. As this ratio is generally chosen by default and scarcely optimized, we intended to investigate the impact of the hydro-alcoholic composition on extract characteristics such as extraction yield, composition profile in selected compounds, and antioxidant/reducing activity such as Folin-Ciocalteu, DPPH, and ORAC. A theoretical determination of rosmarinic (RA) and carnosic (CA) acid solubilities in ethanol:water mixtures was also performed using COSMO-RS and was confronted to experiments. While the best solubilizing solvent (100% ethanol) was also the best extracting solvent for CA, it was not the case with RA since pure ethanol appeared as a poor solvent compared to 30% ethanol which was optimal. Finally, the best antioxidant activities were obtained with 30% ethanol.