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Abstract In this study, we propose an effective strategy for achieving the flexible one organic transistor–one organic memristor (1T–1R) synapse using the multifunctional organic memristor. The dynamics of the conductive nanofilament (CF) in a hydrophobic fluoropolymer medium is explored and a hydrophobic fluoropolymer-based organic memristor is developed. The flexible 1T–1R synapse can be fabricated using the solution process because the hydrophobic fluorinated polymer layer is produced on the organic transistor without degradation of the underlying semiconductor. The developed flexible synapse exhibits multilevel conductance with high reliability and stability because of the fluoropolymer film, which acts as a medium for CF growth and an encapsulating layer for the organic transistor. Moreover, the synapse cell shows potential for high-density memory systems and practical neural networks. This effective concept for developing practical flexible neural networks would be a basic platform to realize the smart wearable electronics.