We show that the properties of photoelectronic synaptic transistors based on films with ordered P3HT polymer chains can be tuned by varying the orientations of the polymer chains with respect to the electrodes. The electrical responses corresponding to displays of synaptic plasticity are studied using a range of electrical and optical stimulations. It is shown that the orientation significantly modulates the properties, demonstrating that the orientation of the polymer film with respect to the electrodes enables a tuning of the synaptic plasticity.