in response to its increase or decrease in activity, which is the biological basis of learning and memory activities at the cellular level. [4,5] In order to meet the great demand for intelligent computing, big data, and web of Things development, the researches on artificial synapse neuromorphic electronic devices have aroused great research enthusiasm, considering the high efficiency of artificial synapse devices mimicking the way the human brain processes complex tasks. [6][7][8][9][10][11] At present, the transistor synapse device has attracted much attention due to its three-terminal structure with greater modulation flexibility. [12][13][14][15][16][17][18] In transistor synapse device, modulated physical quantities (such as conductance, current, etc.) like synaptic weight updating and synaptic devices can be used to implement basic and important presynaptic and postsynaptic information transmission and effectively simulate short-term, long-term memory, frequency dependence, long-term potentiation and long-term depression of biological synapses. [19][20][21][22] As a key component of organic electronic devices, organic transistor has a broad development prospect in wearable electronic devices, human electronic skin, scrollable touch display, and other new applications. [23][24][25][26][27][28] Unlike inorganic synapses, organic materials have great advantages in mass manufacturing, large area, mechanical flexibility, and solution processability. [29][30][31][32] These peculiarities, combined with the tunable flexibility of three terminals, make organic neuromorphic transistors stand out in the field of neuromorphic computing. [33][34][35] However, organic synaptic transistors have many inherent drawbacks, for instance, small conductivity changes, low storage performance, asymmetric weight updating, as well as fewer conductivity states. [36,37] In order to overcome these limitations, researchers have carried out research to improve the performance of organic synaptic devices in the aspects of materials, interface engineering and blend composite. [38][39][40] The vertical organic transistor (VOT) changes the conductive channel from the traditional horizontal to vertical, and the channel layer thickness is the channel length of the device, which effectively overcomes the performance limitation of traditional horizontal channel structure. Compared to traditional transistors, VOTs benefit from extremely short channels, providing a platform for fast switching speeds and ultra-high output current density. [41,42] In addition, the planar charge transfer in traditional transistors is affected by the morphology of the semiconductor/insulator interface, while for VOTs, because the channel between source Neuromorphic technology is the next stage in the evolution of high-performance computing, with its ability to dramatically improve data processing and learning. Hence, the exploration of synaptic electronic devices with multiple excitation modes is the main area of concern. In this work, a vertical organic ferroelectri...