Ferroelectric polymers have drawn a lot of research concerns recently due to their lightness, mechanical flexibility, conformability, and facile processability. Remarkably, these polymers can be used to fabricate biomimetic devices, such as artificial retina or electronic skin, to realize artificial intelligence. The artificial visual system behaves as a photoreceptor, converting incoming light into electric signals. The most widely studied ferroelectric polymer, poly(vinylidene fluoride-trifluoroethylene) [P(VDF-TrFE)], can be used as the building block in this visual system to implement synaptic signal generation. There is a void in computational investigations on the complicated working picture of P(VDF-TrFE)-based artificial retina from a microscopic mechanism to a macroscopic mechanism. Therefore, a multiscale simulation method combining quantum chemistry calculations, first-principles calculations, Monte Carlo simulations, and the Benav model was established to illustrate the whole working principle, involving synaptic signal transduction and consequent communication with neuron cells, of the P(VDF-TrFE)-based artificial retina. This newly developed multiscale method not only can be further applied to other energy-harvesting systems involving synaptic signals but also would be helpful to build microscopic/macroscopic pictures within these energy-harvesting devices.