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Recent advances in the fabrication of neuromorphic electronic devices using biomaterials have received increasing attention for their prospect in biologically compatible and “green” electronic devices. Here, we proposed a novel electric-double-layer (EDL) synaptic transistor gated with Li-doped natural gelatin membranes, demonstrating larger capacitance at low frequency and extremely strong electrostatic modulation behavior. Experimental results have shown that a concentration of 2 wt. % Li-doping can obtain better electrical performance of EDL synaptic transistor. Ion/Ioff of 4.86 × 105 and threshold voltage of 0.68 V were obtained. Meanwhile, some important synaptic functions such as excitatory postsynaptic current, paired-pulse facilitation, and high-pass filtering characteristic have been successfully implemented. As a result, it can be inferred that the proposed gelatin-based natural polymer EDL electrolyte has demonstrated potential applications in “green” neuromorphic platforms.