Mesomorphic arylsulfonamide derivatives containing four long alkyl chains and polar groups (fluoro, cyano or amino) have been synthesized and characterized by polarized optical microscopy, differential scanning calorimetry, and X‐ray diffraction on the mesophase. Studies of the supramolecular organization of these molecules have allowed a better understanding of the noncovalent driving forces (dipole···dipole and hydrogen‐bonding interactions) responsible for the self‐assembly, which is mainly due to the presence of the polar groups.

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