Abstract: Designing spatial and structural features from the molecular to macroscopic scale has become one of the most important topics in materials science in recent years. Covalent organic frameworks (COFs) are a class of crystalline porous materials composed of two- or three-dimensional network structures connected by covalent bonds. These materials exhibit high specific surface area, well-defined pore channels, clear structural designability, and excellent stability. Its tunable chemical structure and high crystallinity are expected to provide potential solutions for improving the uniformity of resistance change performance, device stability, continuous resistance variation and low-power flexible edge computing. This article reviews the recent progress of COFs materials in terms of structure, device fabrication, and performance research. It also discusses the key scientific issues that need to be addressed urgently and the future development directions. It is expected that, with technological breakthroughs in three areas—large-area high-quality film fabrication, direct characterization of resistive switching mechanisms, and integration of device arrays, COFs-based materials will emerge as a leading candidate for transitioning from cutting-edge laboratory materials to next-generation nonvolatile memory and neuromorphic computing. The overall development prospects would be very broad.