Abstract In this era of artificial intelligence and Internet of Things, emerging new computing paradigms such as in‐sensor and in‐memory computing call for both structurally simple and multifunctional memory devices. Although emerging two‐dimensional (2D) memory devices provide promising solutions, the most reported devices either suffer from single functionalities or structural complexity. Here, this work reports a reconfigurable memory device (RMD) based on MoS 2 /CuInP 2 S 6 heterostructure, which integrates the defect engineering‐enabled interlayer defects and the ferroelectric polarization in CuInP 2 S 6 , to realize a simplified structure device for all‐in‐one sensing, memory and computing. The plasma treatment‐induced defect engineering of the CuInP 2 S 6 nanosheet effectively increases the interlayer defect density, which significantly enhances the charge‐trapping ability in synergy with ferroelectric properties. The reported device not only can serve as a non‐volatile electronic memory device, but also can be reconfigured into optoelectronic memory mode or synaptic mode after controlling the ferroelectric polarization states in CuInP 2 S 6 . When operated in optoelectronic memory mode, the all‐in‐one RMD could diagnose ophthalmic disease by segmenting vasculature within biological retinas. On the other hand, operating as an optoelectronic synapse, this work showcases in‐sensor reservoir computing for gesture recognition with high energy efficiency.

2D Reconfigurable Memory Device Enabled by Defect Engineering for Multifunctional Neuromorphic Computing