The optical and cost transport properties of natural semiconductors are strongly influenced by their morphology and molecular buildings. Right here we report the affect of a molecular template technique on anisotropic management by way of weak epitaxial development of a semiconducting channel for a dinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]thiophene (DNTT)/para-sexiphenyl (p-6P) heterojunction. The goal is to enhance cost transport and trapping, to allow tailoring of visible neuroplasticity. The proposed phototransistor units, comprising a molecular heterojunction with optimized molecular template thickness, exhibited a wonderful reminiscence ratio (ION/IOFF) and retention traits in response to gentle stimulation, owing to the improved orientation/packing of DNTT molecules and a good match between the LUMO/HOMO ranges of p-6P and DNTT. The most effective performing heterojunction reveals visible synaptic functionalities, together with an especially excessive pair-pulse facilitation index of ∼206%, ultralow vitality consumption of 0.54 fJ, and zero-gate operation, underneath ultrashort pulse gentle stimulation to imitate human-like sensing, computing, and reminiscence features. An array of heterojunction photosynapses possess a excessive diploma of visible sample recognition and studying, to imitate the neuroplasticity of human mind actions via a rehearsal studying course of. This examine offers a information to the design of molecular heterojunctions for tailoring high-performance photonic reminiscence and synapses for neuromorphic computing and synthetic intelligence techniques.