Covalent　organic　frameworks　(COFs)　have　emerged　as　a　compelling　class　of　materials　for　active　layers　in　memristors,　yet　the　determinants　of　their　electrical　properties　and　effective　tuning　strategies　remain　elusive.　Herein,　the　study　unveils　two　novel　pyrene-based　COFs　(Py-COFs)-the　one-dimensional　(1D)　H-Py-BT　COF　and　the　two-dimensional　(2D)　Py-BT　COF-crafted　with　structural　kinship　yet　divergent　dimensionalities　via　tailored　pyrene　monomer　connectivity.　The　effect　of　structural　and　dimensional　disparities　on　memristive　device　performance　and　image　recognition　precision　is　systematically　investigated.　Notably,　the　1D　H-Py-BT　COF　harnesses　weak　in-plane　and　interlayer　hydrogen　bonding　interactions　to　enhance　charge　separation　and　promote　directional　electron　transport.　This　unique　configuration　enables　devices　fabricated　with　the　1D　H-Py-BT　COF　(101　nm　thick)　to　deliver　exceptional　performance,　evidenced　by　a　high　ON/OFF　current　ratio　(approximate　to　103.7)　and　an　image　recognition　accuracy　of　76%,　outperforming　those　based　on　the　2D　Py-BT　COF.　These　findings　underscore　the　pivotal　role　of　COF　dimensionality　and　molecular　interactions　in　dictating　device　functionality,　offering　valuable　insights　for　advancing　COF-based　memristive　technologies.