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Interfacial properties of single-crystalline CeO2 high-k dielectrics directly grown on Si (111) were investigated by comparing metal–insulator–semiconductor field-effect transistors (MISFETs) without any interfacial layer [(w/o-IL); direct growth of CeO2 on Si] and those with an interfacial layer (w-IL). FET characteristics, such as the drain current and the S factor, for the w/o-IL MISFET were much worse than those for the w-IL MISFET. The in-gap states attributed to the oxygen defects were detected in the CeO2 directly grown on Si by x-ray photoelectron spectroscopy measurements. The large interface state density induced by the oxygen defects at the CeO2/Si interface may deteriorate the w/o-IL MISFET performances.