Mimicking synaptic functions in hardware devices is a crucial step in realizing brain-like computing beyond the von Neumann architecture. 1D nanomaterials with spatial extensions of a few μm, similar to biological neurons, gain significance given the ease of electrical transport as well as directionality. Herein, we report a two-terminal optically active device based on 1D supramolecular nanofibres consisting of CS (coronene tetracarboxylate) and DMV (dimethyl viologen) forming alternating D–A (donor–acceptor) pairs, emulating synaptic functions such as the STP (short-term potentiation), LTP (long-term potentiation), PPF (paired-pulse facilitation), STDP (spike-time dependent plasticity) and learning–relearning behaviors. In addition, an extensive study on the less explored Ebbinghaus forgetting curve has been carried out. The supramolecular nanofibres being light sensitive, the potential of the device as a visual system is demonstrated using a 3 × 3 pixel array.