Abstract
Van der Waals organic/inorganic heterostructures in the two-dimensional (2D) limit with extensive structural tunability will advance the development of artificial solids with tailored functionalities. Recent breakthroughs in several types of 2D organic materials, including molecular monolayer films, 2D polymers, covalent-organic frameworks, and metal oxide frameworks, have greatly enriched the design possibilities of heterostructures with inorganic 2D materials. This review provides a timely summary of the latest advances in synthesis approaches toward advanced organic/inorganic heterostructures, answers the fundamental questions regarding the interfacial interactions in the 2D limit, and further highlights the uses of such organic/inorganic heterostructures in advanced transistors, optoelectronics, neuromorphic, and other multifunctional devices with unique capabilities.