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This work mainly deals with the segregating behaviors of Sc and the growth of unique primary Al 3 Sc in Al-Sc alloys prepared by molten salt electrolysis. The alloys contain 0.23–1.38 wt%Sc where Sc segregation is observed. It is found that a high current density and long electrolysis time are in favor of high Sc content, and so do the high temperature and the addition level of Sc 2 O 3. Sc content at the edge of Al based alloy (average Sc content: 0.75 wt%) can be as high as 1.09 wt%, while it is merely 0.24 wt% at the central area. The cooling rates have a strong impact on the morphology and particle size of primary Al 3 Sc, but a weak influence on Sc segregation. The cusped cubic and dendritic primary Al 3 Sc can precipitate in the prepared Al-Sc alloys. In a slightly hypereutectic Al-0.67 wt%Sc alloy, a large and cusped dendrite grows from the edge into the center. The primary and secondary dendritic arms can be as long as 600 and 250 μm, respectively. The Sc segregating behaviors in Al-Sc alloys is due to the mechanism controlled by the limited diffusion rate of Sc in liquid Al. This can involve the establishment of a near spherical discharge interface between liquid Al and the electrolyte. The Sc rich layer near Al-molten salt interface may provide the potential primary nuclei and sufficient Sc atoms for the growth of large dendritic primary Al 3 Sc. [ABSTRACT FROM AUTHOR]