Solvent‐Driven Synthesis of DNA‐Based Liquid Crystalline Organogels with Extraordinary Stretchability, Self‐Healing, and Higher‐Order Structural Assembly

Abstract The fabrication of liquid crystalline (LC) organogel via supramolecular interactions between Deoxyribonucleic acid (DNA) and lyotropic cationic surfactant containing cyanobiphenyl moiety is reported. The fabricated organogel endows dominantly viscous behavior in dimethyl sulfoxide (DMSO) and elastic behavior in n‐propanol (n‐PrOH), respectively. By judiciously controlling the viscosity, DMSO organogels can be drawn to form a fiber with an elongation of up to 4.6 × 10³%, emphasizing extraordinary stretchability. Higher‐order structures, such as yarn and a co‐alignment matrix for anisotropic particles, can be produced by assembling a single fiber. On the other hand, free‐standing n‐PrOH organogels demonstrate a remarkable storage modulus of 10⁵ Pa and manifest self‐healing properties. Finally, a sustainable method by transforming n‐PrOH gel into an aerogel through critical point drying (CPD), enabling its use as an adsorbent while simultaneously enhancing its reusability is proposed. It is envisaged that these DNA‐based organogels, through conceivable combinations between DNA as a building block and cationic surfactant with functionalities as a counterpart, will contribute to significant progress in DNA‐based multi‐functional organogels.