Intermolecular Hydrogen‐Bond Stabilized 1D Pyrene‐Based Covalent Organic Framework for Advanced Memory Devices and Neuromorphic Computing

Abstract Covalent organic frameworks (COFs) have emerged as a compelling class of materials for active layers in memristors, yet the determinants of their electrical properties and effective tuning strategies remain elusive. Herein, the study unveils two novel pyrene‐based COFs (Py‐COFs)—the one‐dimensional (1D) H‐Py‐BT COF and the two‐dimensional (2D) Py‐BT COF—crafted with structural kinship yet divergent dimensionalities via tailored pyrene monomer connectivity. The effect of structural and dimensional disparities on memristive device performance and image recognition precision is systematically investigated. Notably, the 1D H‐Py‐BT COF harnesses weak in‐plane and interlayer hydrogen bonding interactions to enhance charge separation and promote directional electron transport. This unique configuration enables devices fabricated with the 1D H‐Py‐BT COF (101 nm thick) to deliver exceptional performance, evidenced by a high ON/OFF current ratio (≈10 3.7 ) and an image recognition accuracy of 76%, outperforming those based on the 2D Py‐BT COF. These findings underscore the pivotal role of COF dimensionality and molecular interactions in dictating device functionality, offering valuable insights for advancing COF‐based memristive technologies.