This study investigates the impact of spin-coating speed on the performance of carbon nanotube (CNT)-based optoelectronic synaptic devices, focusing on their long-term memory properties. CNT films fabricated at lower spin speeds exhibited a greater thickness and density compared to those at higher speeds. These denser films showed enhanced persistent photoconductivity, resulting in higher excitatory postsynaptic currents (EPSCs) and the prolonged retention of memory states after UV stimulation. Devices coated at a lower spin-coating speed of 2000 RPM maintained EPSCs above 70% for 3600 s, outperforming their higher-speed counterparts in long-term memory retention. Additionally, the study demonstrated that the learning efficiency improved with repeated UV stimulation, with fewer pulses needed to achieve the maximum EPSC in successive learning cycles. These findings highlight that optimizing spin-coating speeds can significantly enhance the performance of CNT-based synaptic devices, making them suitable for applications in neuromorphic computing and artificial neural networks requiring robust memory retention and efficient learning.