A flexible, low-voltage, and nonvolatile memory device was fabricated by implanting a functional monolayer on an aluminum oxide dielectric surface in a pentacene-based organic transistor. The monolayer-forming molecule contains a phosphonic acid group as the anchoring moiety and a charge-trapping core group flanked between two alkyl chain spacers as the charge trapping site. The memory characteristics strongly depend on the monolayer used due to the localized charge-trapping capability for different core groups, including the diacetylenic (DA) unit as the hole carrier trap, the naphthalenetetracarboxyldiimide (ND) unit as the electron carrier trap, and the one with both DA and ND units present, respectively. The device with the monolayer carrying both DA and ND groups has a larger memory window than that for the one containing DA only and a longer retention time than that for the one containing DA or ND only, giving a memory window of 1.4 V and a retention time around 10(9) s. This device with hybrid organic monolayer/inorganic dielectrics also exhibited rather stable device characteristics upon bending of the polymeric substrate.