A promising approach for implementing biomimetic systems relies on organic electronic devices designed to emulate neural synapses. However, organic artificial synapses face challenges in achieving high yield and robustness, rendering them difficult to use in practical applications. In this work, a high-yield and highly stable bulk heterojunction (BHJ) synaptic device composed of Poly(3-hexylthiophene-2,5-diyl) (P3HT) and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) was fabricated via a simple solution process followed by thermal treatments. The crystallinity of P3HT and the precipitation of PCBM in BHJ films can be controlled by the thermal annealing temperatures. At 80 °C, P3HT reaches its highest crystallinity, while PCBM remains uniformly distributed. This thermal treatment significantly contributes to the fabrication of devices characterized by a high yield rate, reaching 98.43%. Additionally, this device remained operational even after being immersed in deionized water, ethanol, and seawater for 100 h. More importantly, it exhibited high elasticity over a wide temperature range from −90 to 310 °C. Finally, this device was utilized to construct a biomimetic vehicle with autonomous memory learning capabilities. After repeated training, the avoidance time was optimized by 31.4%. The robust P3HT:PCBM artificial synapses hold great promise for advancing the development of biomimetic electronic products in extreme environments.

High-Yield Production of Solution-Processed Highly Robust Organic Artificial Synapses by Thermal Treatments