Two‐Dimensional Covalent Organic Frameworks in Organic Electronics

Abstract Two‐dimensional covalent organic frameworks (2DCOFs) are a unique class of crystalline porous materials interconnected by covalent bonds, which have attracted significant attention in recent years due to their chemical and structural diversity, as well as their applications in adsorption, separation, catalysis, and drug delivery. However, research on the electrical properties of 2DCOFs remains limited, despite their potential in organic electronics. Early studies recognized the poor electrical conductivity of 2DCOFs as a significant obstacle to their application in this field. To overcome this challenge, various strategies have been proposed to enhance conductivity. This review first introduces the concept of computational screening for 2DCOFs and explores approaches to improve their intrinsic conductivity, with a focus on four key aspects: in‐plane and out‐of‐plane charge transport, topology, bandgap, and morphology. It then examines the application of pristine 2DCOFs in organic electronics, including applications in field‐effect transistors, memristors, photodetectors, and chemiresistive gas sensors. We support these strategies with detailed statistical data, providing a comprehensive guide for the design and development of novel 2DCOFs for organic electronics. Finally, we outline future research directions, emphasizing the challenges that remain to be addressed in this emerging area.