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Three‐dimensional (3D) covalent organic frameworks (COFs) are crystalline porous polymers with potential in numerous high‐tech applications, but the linkages involved in their synthesis are still rather limited. Herein, we report novel 3D sp2 carbon‐linked COFs fabricated by the formation reaction of C=C bonds and their application in fluorescence imaging. These new COFs, namely JUC‐580 and JUC‐581,...