AbstractTwo organogelators, CO‐01 and CO‐03, featuring benzimidazole and long‐chain pyridine carboxyamide groups were prepared and their physical properties were fully explored. CO‐01 and CO‐03 are capable of transforming various organic solvents to organogels. The morphologic investigations of these organogels have shown that the supramolecular assemblies, in the forms of fibers and spheres, are readily generated from the aggregates of CO‐01 and CO‐03. The sol–gel interconversion can be readily achieved by tuning the gelator concentration and temperature. By manipulating the redox state of anthraquinone group in CO‐03, the gel–sol transition for the organogels of CO‐03 can be reversibly tuned by either chemical or electrochemical oxidation/reduction reactions. The presence of polarized imidazole and amide N–H groups allows anion‐induced gel collapse. The accompanying colorimetric and ratiometric fluorescent responses of gels CO‐01 and CO‐03 to F− and CN− render these organogelators being sensitive and selective anion probes.