Photo-Stimulated Ferroelectric Memories In article number 2307346, Kanghoon Yim, Young-Jun Yu, and co-workers demonstrate white-light illuminated α-In2Se3 ferroelectric field effect transistors for efficient synaptic memory operation. By spontaneous Fermi level regulation of α-In2Se3 with photogenerated electron-hole pairs, the strengthened built-in electric field within an α-In2Se3 channel allows the superior recognition accuracy of artificial neural networks. This advancement could be invaluable in the forthcoming era of artificial neuromorphic computing.