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2D metal‐organic framework (MOF) film as the active layer show promising application prospects in various fields including sensors, catalysis, and electronic devices. However, exploring the application of 2D MOF film in the field of artificial synapses has not been implemented yet. In this work, we fabricated a novel 2D MOF film (Cu‐THPP, THPP=5,10,15,20‐Tetrakis(4‐hydroxyphenyl)‐21H,23H‐porphine), and further used it as an active layer to explore the application in the simulation of human brain synapses. It shows excellent light‐stimulated synaptic plasticity properties, and exhibits the foundation function of synapses such as long‐term plasticity (LTP), short‐term plasticity (STP), and the conversion of STP to LTP. Most critically, the MOF based artificial synaptic device exhibits an excellent stability in atmosphere. This work opens the door for the application of 2D MOF film in the simulation of human brain synapses. [ABSTRACT FROM AUTHOR]

Owing to their excellent physical and electrical properties, metal–organic framework (MOF) materials with well‐defined supramolecular structures have received extensive research attention. However, the fabrication of large‐area two‐dimensional (2D) MOF films is still a significant challenge. Herein, we propose a novel electrochemical (EC) synthesis method for the preparation of large‐area Cu3(HHTP)2 MOF film on single‐crystal Cu (100) anode. The surface reaction was achieved via charge‐induced molecular assembly. The synthesized MOF film exhibited a high crystalline quality with an electrical conductivity of approximately 0.087 S cm−1, which was around 1000 times larger than the previously reported values for the same material prepared by the interface method. In addition, Cu2(MTCP), Cu3(BTPA)2, and Cu3(TPTC)2 MOF films were synthesized on Cu foil with the same strategy, which confirmed the universality of the proposed method. This controllable EC method can be effectively applied to the industrial‐scale production of 2D MOF films on Cu foil. [ABSTRACT FROM AUTHOR]