The oscillatory retinal neuron (ORN) is a promising technology for achieving in-sensor cognitive image computing without external power. While its operation is based on photoinduced negative differential resistance (NDR) at a graphene/silicon interface to directly convert the incident optical signal into voltage oscillations, the optoelectronic mechanism of the NDR remains elusive. Here, nonadiabatic quantum molecular dynamics simulations show that the interplay of band alignment and charge transfer rates of photoexcited carriers at varying applied voltages gives rise to NDR at a graphene/silicon interface under illumination. Such intrinsic NDR at an interface, along with extrinsic circuit-level factors, could enable the much needed rational design of desired image computing functionality of ORN devices in the era of ubiquitous AI on edge devices.