cube (HMC), [5] high bandwidth memory (HBM), [6,7] and 3D monolithic integration, [8] have been successively developed and achieved some success, the challenge of latency and energy consumption caused by massive data transmission still remains. Therefore, it is urgently necessary to enhance the information interaction capability by improving the architectural relationship between processing and memory units.The emergence of non-von-Neumann architecture solves the problem of the separation of processing and memory units, and alleviates the impact of bus bandwidth on computing efficiency. As a non-Von Neumann architecture, in-memory computing has been considered to be one of the future mainstream trends of hardware implementation for AI algorithms, [9] such as machine learning and deep learning. In-memory computing, where calculations are carried out in situ within each memory unit, [10] has massive parallelism and distributed computing characteristic through integrating millions of memory devices in a crossbar array (Figure 1), analogous to the neurobiological system. [11] Thus, it can radically subvert the von Neumann architecture and achieve the fusion of data processing and storage, thereby totally eliminating the latency and energy loss associated with data access. For enabling this computational architecture, new material systems and highperformance memory devices are highly pursued.2D layered materials refer to the material family that held together by strong in-plane chemical bonds and relatively weak out-of-plane van der Waals interactions, and have attracted worldwide attention due to their unique structure and physical properties. [12][13][14][15][16][17][18][19][20][21] On the one hand, the atomically thin thickness of 2D layered materials provide a significant advantage in achieving high-density integration and low-power operation of high-performance devices. [22][23][24][25][26][27][28] On the other hand, their dangling-bond-free surface and planar structure make them not only compatible with traditional wafer technology, but also can be stacked on top of each other unrestricted by lattice mismatch. Thus, varieties of available 2D layered materials with different electrical properties, such as graphene, transition metal dichalcogenides (TMDs, including MoS 2 , WSe 2 , MoTe 2 , etc.), black phosphorus (BP) and hexagonal boron nitride (h-BN), could be arbitrarily assembled to create a wide range of artificial van der Waals heterostructures (vdWHs) with wholly new functionalities that unavailable in the individual material. [29][30][31][32][33] For example, stable data storage can be realized with the aid of potential barrier formed in vdWHs. [34][35][36][37][38][39] Additionally, It is predicted that the conventional von Neumann computing architecture cannot meet the demands of future data-intensive computing applications due to the bottleneck between the processing and memory units. To try to solve this problem, in-memory computing technology, where calculations are carried out in situ within each nonv...