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A nonvolatile organic transistor memory device was developed using layer-by-layer assembly of 3-aminopropyltriethoxysilane (APTES) and solution-processed, reduced graphene oxide (rGO) as the charge trapping layer on flexible substrates. Reduction of graphene oxide and successful adsorption of the rGO on APTES-covered substrates were confirmed. The organic memory devices based on rGO exhibited reliable programmable memory operations, confirmed by program/erase operations, data retention, and endurance properties. These methods can potentially play a significant role in the fabrication of next-generation flexible nonvolatile memory devices based on graphene materials.