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We proposed a synaptic transistor gated using a Ta₂O₅ barrier-layered organic chitosan electric double layer (EDL) applicable to a micro-neural architecture system. In most of the previous studies, a single layer of chitosan electrolyte was unable to perform lithography processes due to poor mechanical/chemical resistance. To overcome this limitation, we laminated a high-<i>k</i> Ta₂O₅ thin film on chitosan electrolyte to ensure high mechanical/chemical stability to perform a lithographic process for micropattern formation. Artificial synaptic behaviors were realized by protonic mobile ion polarization in chitosan electrolytes. In addition, neuroplasticity modulation in the amorphous In–Ga–Zn-oxide (a-IGZO) channel was implemented by presynaptic stimulation. We also demonstrated synaptic weight changes through proton polarization, excitatory postsynaptic current modulations, and paired-pulse facilitation. According to the presynaptic stimulations, the magnitude of mobile proton polarization and the amount of weight change were quantified. Subsequently, the stable conductance modulation through repetitive potential and depression pulse was confirmed. Finally, we consider that proposed synaptic transistor is suitable for advanced micro-neural architecture because it overcomes the instability caused when using a single organic chitosan layer.