This paper reports on the development of suitable ethanol-based suspensions, using polyelectrolytes, for the controlled shaping of functionally graded Al2O3/ZrO2 materials by means of electrophoretic deposition. Literature reports mainly focus on the relationship between the optimum amount of charging agent, the suspension stability and the electrophoretic deposition behaviour. However, due to the complexity of physical and chemical phenomena involved, a general rule cannot be established. Aqueous suspensions of Al2O3 and ZrO2 powders, stabilized with a polyelectrolyte are well understood. Because aqueous suspensions present some limitations in the EPD process, due to the electrolysis of water at higher voltages, an organic environmentally friendly solvent with high dielectric constant is investigated. The minimum amount and type of charging agent and polyelectrolyte as well as their addition sequence is investigated by means of zeta potential measurements. The usefulness of the investigated suspensions is evaluated by shaping symmetrically graded alumina-zirconia discs, using a macroscopic model for the EPD process that allows to predict the final gradient in the sintered disc based on the powder characteristic, suspension characteristic and experimental EPD, parameters.