In this study, Taguchi design method with L9 orthogonal array has been used to optimize the initial thickness and pre-aging parameters (temperature and time) for the mechanical properties of Al-0.2 wt.% Sc alloy heavily deformed by accumulative roll bonding (ARB) up to ten cycles. Analysis of variance was performed on the measured data and signal-to-noise ratios. It was found that the pre-aging temperature has the most significant parameter affecting the mechanical properties by percentage contribution of 64.51%. Pre-aging time (19.29%) has the next most significant effect, while initial thickness (5.31%) has statistically less significant effect. In order to confirm experimental conclusions, verification experiments were carried out at optimum working conditions. Under these conditions, the yield strength was 6.51 times higher and toughness was 6.86% lower compared with the starting Al-Sc material. Moreover, mean grain size was decreased to 220 nm by setting the control parameters, which was the lowest value obtained in this study. It was concluded that the Taguchi method was found to be a promising technique to obtain the optimum conditions for such studies. Consequently, by controlling the parameter levels, the high-strength and high-toughness Al-Sc samples were fabricated through pre-aging and subsequent ARB process.