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COSMO-based process simulations using Aspen Plus and Aspen HYSYS were systematically applied to the conceptual design of the two main unit operations commonly proposed to separate aromatic and aliphatic hydrocarbons with ionic liquids (ILs) as extracting solvents; the extraction itself and the vacuum distillation for regenerating the ionic liquid. By the first time, multi-component (up to 28 components) “real” mixture feeds were taken into account to model the naphtha in the process design. Binary model (n-hexane + benzene, n-heptane + toluene, n-octane + ethylbenzene, n-octane + m-xylene) mixture feeds were also considered to validate the computational procedure. Nine different ionic liquids and mixtures of them, (IL–IL) mixtures, were selected as extracting solvents. Ionic liquids were introduced in the process simulations as (pseudo)components and the COSMOSAC property model was used for …