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Time-resolved observation of synchrotron radiation was utilized to investigate the formation behavior of Fe-/Mn-containing intermetallic phases in the Al-Si casting alloys as functions of solute elements and cooling rate. For low Fe-/Mn-containing alloys, the primary o-AIFeMnSi phase was detected to crystallize from a liquid state, followed by the eutectic reaction regardless of cooling rate in this experimental range. During the eutectic reaction, the formation of the eutectic β- Al5FeSi phase was clearly observed to proceed in the inter-dendritic region after the emergence of dendritic α-Al in the Al-Si alloys. It was also observed that the average microstructural size of the specimen was noticeably reduced with the increasing cooling rate. For high Fe-ZMn-containing alloys, however, two primary phases of α-AlFeMnSi and α-AlFeSi were clearly seen at the low cooling rate regime, and three primary phases of β-Al5FeSi, α-AlFeMnSi, and α-AlFeSi were recorded at the high cooling rate regime. Both primary crystallization systems of two different cooling rate regimes were followed by successive eutectic reactions to form an eutectic microstructure of α-Al and β-Al5FeSi, of which microstructural size was less dependent on the cooling rate compared to that of the low Fe-/Mn-containing alloys.