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This research presents a multi-layer optimization framework for hybrid energy storage systems (HESS) for passenger electric vehicles to increase the battery system's performance by combining multiple cell chemistries. Specifically, we devise a battery model capturing voltage dynamics, temperature and lifetime degradation solely using data from manufacturer datasheets, and jointly optimize the capacity distribution between the two batteries and the power split, for a given drive cycle and HESS topology. The results show that the lowest energy consumption is obtained with a hybrid solution consisting of a NCA-NMC combination, since this provides the best trade-off between efficiency and added weight.