Covalent organic frameworks (COFs) are promising active mediums for high‐performance data storage devices stemming from their high crystallinity, ordered porous channels, predetermined topology, and rigid architectures, while relative studies are still limited. Here, two COFs (i.e., COF‐EtD and COF‐EtA)‐based resistive‐switching memory devices are proposed to demonstrate the impact of intramolecular hydrogen bonding interactions, both of which exhibit nonvolatile write‐once‐read‐many (WORM) memory characteristics. Comparatively, COF‐EtD with the hydroxyl motif decoration illustrated a lower SET voltage (i.e., turn‐on voltage) and a higher ON/OFF current ratio as well as exceptional high‐temperature endurance and solvent resistance. Mechanism explorations suggest that the resistance‐switching behavior of COF‐EtD may be controlled by the synergistic effect of space‐charge‐limited current and conductive filaments. This finding is the first example of simply varying the functional group of COFs to regulate the WORM resistive switching behavior, providing some inspiration for the advancement of electronic memories and positively contributing to the realization of high endurance and high‐density electric storage materials.