Emulation of advanced synaptic functions of the human brain with electronic devices contributes an important step toward constructing high-efficiency neuromorphic systems. Ferroelectric materials are promising candidates as synaptic weight elements in neural network hardware due to their controllable polarization states. However, the increased depolarization field at the nanoscale and the complex fabrication process of the traditional ferroelectric materials hamper the development of high-density, low-power, and highly sensitive synaptic devices. Here, we report the implementation of twodimensional (2D) ferroelectric α-In 2 Se 3 as an active channel material to emulate typical synaptic functions. The α-In 2 Se 3-based synaptic device features multimode operations, enabled by the coupled ferroelectric polarization under various voltage pulses applied at both drain and gate terminals. Moreover, the energy consumption can be reduced to~1 pJ by using high-κ dielectric (Al 2 O 3). The successful control of ferroelectric polarizations in α-In 2 Se 3 and its application in artificial synapses are expected to inspire the implementation of 2D ferroelectric materials for future neuromorphic systems. K E Y W O R D S 2D ferroelectrics, artificial synapse, high-κ dielectric, multimode operations, α-In 2 Se 3 1 | INTRODUCTION Over the past few decades, computers based on the conventional von Neumann architecture have achieved great success in performing arithmetic operations, leading to the revolution of information technology. 1 However, the physically separated logic and memory blocks, known as von Neumann bottleneck, inevitably limit the computational efficiency and speed as well as the scalability of the architecture. 2,3 Inspired by human brain, neuromorphic