Neuromorphic devices encounter constraints associated with complementary metal–oxide–semiconductor technology, such as intricate electronics and high power consumption. Recently, solid polymer electrolytes (SPE) have gained attraction in electronic devices for constructing artificial synapses, primarily due to their low-voltage operation enabled by ion-assisted signal transmission. This study presents a two-terminal artificial synapse fabricated using fluorine graphdiyne (F-GDY) synthesized through chemical vapor deposition and ion-doped SPE. The device architecture consists of Au/SPE/F-GDY/Si, which operates by ion migration induced by external potential pulses. Electrical measurements are conducted to depict the synaptic plasticity of the devices. Among devices employing different ion-doped SPEs (Li-SPE, Na-SPE, K-SPE, and Ca-SPE), the one utilizing Li-SPE demonstrates the highest synaptic weight. This is attributed to the superior Li+ ion storage capacity of F-GDY; hence, Li-SPE/F-GDY was chosen for in-depth examinations of synaptic activity presenting long-term potentiation, short-term depression, and pair-pulse facilitation. The device has good durability and stability and can respond to low action potential with power consumption at the pJ level. Furthermore, Modified National Institute of Standards and Technology simulations reveal its learning and pattern recognition capability with 91.3 % accuracy after 10 training epochs. Finally, flexible substrate-based SPE/F-GDY devices integrated with gate electrodes were fabricated to record physiological signals, showing promise for in-sensing applications. This work shows the potential of F-GDY/Li-SPE devices for low-power neuromorphic computing, though real-time parallel processing and multimodal integration (e.g., visual, auditory) remain unexplored. However, the biocompatibility and efficient ion-assisted transmission of F-GDY suggest promising future applications in these areas.