Due to the potential applications in optoelectronic memories, optical control of ferroelectric domain walls has emerged as an intriguing and important topic in modern solid‐state physics. However, its device implementation in a single ferroelectric, such as conventional BaTiO3 or PZT ceramics, still presents huge challenges in terms of the poor material conductivity and the energy mismatch between incident photons and ferroelectric switching. Here, using the generation of photocurrent in conductive α‐In2Se3 (a van der Waals ferroelectric) with a two‐terminal planar architecture, the first demonstration of optical‐engineered ferroelectric domain wall in a non‐volatile manner for optoelectronic memory application is reported. The α‐In2Se3 device exhibits a large optical‐writing and electrical‐erasing (on/off) ratio of >104, as well as multilevel current switching upon optical excitation. The narrow direct bandgap of the multilayer α‐In2Se3 ferroelectric endows the device with broadband optical‐writing wavelengths greater than 900 nm. In addition, photonic synapses with approximate linear weight updates for neuromorphic computing are also achieved in the ferroelectric devices. This work represents a breakthrough toward technological applications of ferroelectric nanodomain engineering by light. An optically engineered ferroelectric domain wall in a layered ferroelectric is demonstrated for optoelectronic memory applications. The device exhibits a large optical‐writing and electrical‐erasing ratio of >104, as well as multilevel current switching upon optical excitation. The optical‐writing wavelength can be greater than 900 nm. Photonic synapses with approximate linear weight updates for neuromorphic computing are also achieved in such devices.