The　rapid　evolution　of　neuromorphic　devices　seeks　to　bridge　biological　neural　networks　and　artificial　systems,　enabling　energy-efficient　and　scalable　computing　for　next-generation　artificial　intelligence.　Herein,　we　introduce　methyl-engineered　one-dimensional　covalent　organic　framework　(1D　COF)-based　memristors　as　a　transformative　platform　for　reconfigurable　neuromorphic　computing.　The　incorporation　of　methyl　groups　enhances　localized　polarization　effects　within　the　COF　framework,　effectively　mitigating　random　Ag+　migration/diffusion　and　stabilizing　conductive　filament　morphology.　This　strategic　modification　yields　devices　with　exceptional　multilevel　storage　capabilities,　exhibiting　superior　stability,　linearity,　and　reproducibility.　Moreover,　the　highly　ordered　architecture　and　customizable　chemical　environment　of　the　methyl-functionalized　1D　COF　allows　for　precise　control　over　resistive　switching　behaviors,　facilitating　the　emulation　of　synaptic　functions　and　the　development　of　artificial　neural　network　architectures.　Demonstrating　exceptional　performance　in　neuromorphic　tasks　such　as　high-accuracy　image　recognition,　these　devices　showcase　significant　promise　as　the　foundation　for　energy-efficient,　next-generation　neuromorphic　computing　systems.　©　2025　American　Chemical　Society.