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Abstract Atomic layer infiltration technology allows the formation of a nanometer-thick polymer-inorganic hybrid barrier layer in polymer material for flexible organic light-emitting diode (OLED) displays. In this study, according to transmission electron microscopy and secondary-ion mass spectrometry analysis results under various process conditions, a compact polymer-inorganic hybrid nanolayer was successfully formed in a polymer and good barrier performance was revealed with a low water vapor transmission rate under optimal process conditions. Additionally, through gas chromatography-mass spectrometry measurements after ultra-violet radiation testing, polymer out-gassing decreased compared to bare polymers. Based on barrier properties, the polymer with a polymer-inorganic hybrid barrier nanolayer was applied to a flexible OLED display as a substrate. During storage tests and folding tests, the flexible OLED display exhibits good reliability and better flexibility compared to those with an inorganic barrier layer. These results confirm that the polymer-inorganic hybrid nanolayer is suitable for barrier layer formation in flexible OLED displays.