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.　©　2023　Wiley-VCH　GmbH.