As a kind of structurally designable, nanoscale controllable, and performance optimizable materials, metal-organic frameworks (MOFs), consisting of organic ligands and metal nodes, have been widely studied as promising materials in a lot of fields over the last two decades, such as sensors, drug delivery, gas separation and storage, catalysis, and so on. [1] However, compared to these mature applications, the adoption of MOFs in emerging areas, such as information storage and processing, is relatively less. [1c,2] In order to expand the applied range of MOFs in new areas, designing and synthesizing new structure MOFs with novel properties, such as conducting and semiconducting characteristics, was recently used. [1c,3] The synthesis of new structure MOFs will lead to the relative high experimental cost and more complex synthesis process. Therefore, expanding the application of the pre-existing MOFs with high performance in emerging areas may be a more effective choice. In this information explosion era, data storage and processing is one of the most significant research field, and various functional materials have been used to develop high performance information storage and processing devices. [4] Up to now, MOFs have been used as active layer for developing nonvolatile memory (NVM), especially resistive random access memory (RRAM), [1c,5] which has been identified as one of the most potential developing direction for future non volatile data storage technique. [6] Moreover, compared with bulk MOFs, 2D MOFs show more attractive performance because they have ultrathin thickness, larger specific surface area, and more highly accessible active sites, and have attracted lots of research interest in the field of sensors, energy conversion and storage, biomedicine, gas separation, and electronic devices. [7] In these 2D MOF materials, M-TCPP (M: metal; TCPP: tetrakis(4carboxyphenyl)porphyrin) nanosheets have been used in biological detection, photocatalysis, RRAM, and other fields due to their simple synthetic process, uniform size, and proper thickness. [8,9] Due to the low information communication rate between central processing unit and main memory, the traditional von Two-dimensional (2D) metal-organic frameworks (MOFs) are widely used in a variety of mature applications, including catalysis, drug delivery, and sensors. Based on their highly accessible active sites, 2D MOFs are expected to be good charge trapping elements. Using 2D MOF, Zn-TCPP (TCPP: tetrakis(4-carboxyphenyl)porphyrin), as charge trapping materials by a simple solution process, a three-terminal synaptic device which can realize the learning functions and signal transmission simultaneously is firstly fabricated. The as-fabricated synaptic device exhibits ambipolar charge carrier trapping performance, large current on /current off ratio (>10 3) and excellent endurance (500 cycle times). Moreover, the common biological synaptic behaviors, including postsynaptic current under different temperature, pulse duration time and pulse voltage, paired-pulse...