cells, [11] and memory. [12,13] Recently, vdWs heterostructure-based nonvolatile optical memory have been investigated for broad potential applications in imaging sensors, [14] logic gates, [15] optoelectronic demodulators, [16] and synaptic devices for neuromorphic systems. [17,18] These 2D vdWs materials and their hybrids are considered to be an ideal platform for nonvolatile optical memory owing to their strong light-matter interactions [19][20][21] and significant photogenerated charge trapping derived from their very large surface-to-volume ratio. [22][23][24] In addition, the mechanical strength and atomic thickness of 2D vdWs materials allow for device miniaturization in flexible and wearable optoelectronics. [25][26][27] The demonstration of 2D vdWs materials-based optical memory in the FETs of few-layer copper indium selenide (CuIn 7 Se 11 ) has been reported [14] along with hybrids of graphene/MoS 2[5] on a silicon substrate. These devices exhibit low optical switching on/off ratios (<1 [5] and ≈10 [14] ), high off-currents (≈400 µA [5] and 20 pA [14] ), and short retention times (50 s [14] ), preventing their use in high quality image sensors and multilevel storage devices.Using oxygen plasma treatments to create more charge trap sites at SiO 2 surface, monolayer MoS 2 -FET-based optical memory on silicon substrate has exhibited a long retention time of ≈10 4 s. [28] However, the data storage capacity of eight levels of the material remains limited for practical applications due to moderate switching on/off ratio of ≈4700. Importantly, the memory function of these devices relies on charge trapping of photoexcited carriers in defects and impurities on either the surface or material/SiO 2 interface. [5,28] This results in short retention times and sensitivity to environmental factors. A charge trapping layer acting as a floating gate, instead of charge trapping at the materials/SiO 2 interface, can be introduced via gold nanoparticle/crosslinked poly(4-vinylphenol)/MoS 2 heterojunction-FETs, which significantly increase both the switching on/off ratio (≈10 6 ) and retention time (>10 4 s). [29] Similarly, by storing charge in the hexagonal boron nitride (h-BN) dielectric layer, the WSe 2 /h-BN-FET-based optical memory on silicon also exhibited a high on/off ratio of 1.1 × 10 6 , realizing a data storage capability of up to 128 distinct states. [30] Despite the long retention time and high on/off ratios of the recently developed vdWs heterostructure-based optical memory 2D van der Waals (vdWs) heterostructures exhibit intriguing optoelectronic properties in photodetectors, solar cells, and light-emitting diodes. In addition, these materials have the potential to be further extended to optical memories with promising broadband applications for image sensing, logic gates, and synaptic devices for neuromorphic computing. In particular, high programming voltage, high off-power consumption, and circuital complexity in integration are primary concerns in the development of three-terminal optical memory devices....