large extent of an isotropic solvent, water in many cases, are more difficult to align in principle. Second, less attention has been paid to developing alignment layers for lyotropic liquid crystals. However, LCLCs, aqueous solutions of aggregates of (often biocompatible) polar organic molecules, [8][9][10][11] have been recognized as a useful link between living organisms and photonics, which can be used, for example, for biosensing. [12] Thus, LCLC alignment techniques based on rubbing, rubbed polymer layers, or patterned substrates have been studied, as well. [13][14][15][16] Recently, aligning interactions between thermotropic and lyotropic liquid crystals have been reported. For example, uniformly aligned layers formed by drying a lyotropic solution of deoxyribonucleic acid (DNA) or another lyotropic liquid crystal were fabricated and found to be suitable for controlling the alignment of a thermotropic liquid crystal, which can then be used as an electrooptic light valve. [17][18][19] Inspired by this recent progress, we developed the new alignment technique for LCLCs further and describe here how it can be applied, when one of the solid substrates is replaced by a flexible foil made of Mylar film, an anisotropic polyethylene terephthalate film, which has been described earlier. [20,21] In the experiments described in the following, uniformly aligned films are prepared from a LCLC without rubbing or brushing. For this purpose, an aqueous solution containing either 15% (by weight) disodium cromoglycate (DSCG, Figure S1, Supporting Information) or 8% DNA sodium salt from herring testes (herring DNA) is confined between a silica substrate and Mylar film. After about 10 min, the LCLC is found to be uniformly aligned and free of defects. Subsequently, the polymer film is removed and the water of the LCLC is allowed to evaporate, which results in an anisotropic solid film spread on the substrate. The orientational order parameter of this film and the orientational order parameter of a thermotropic liquid crystal aligned by the film are measured.Aqueous solutions of DSCG show the well-known liquid crystalline mesophases, which have been described previously. [1][2][3][4]22] A nematic (N) phase appears for DSCG concentrations between ≈9% and ≈28% by weight, while a columnar (M) phase is observed for concentrations between ≈17% and ≈33%, depending on the pH-value and salt concentration. [23] A Uniformly aligned layers made of disodium cromoglycate (DSCG) or doublestranded deoxyribonucleic acid (DNA) are fabricated. For this purpose, a thin liquid layer of a lyotropic chromonic liquid crystal made of DSCG and water or an aqueous solution of DNA is sandwiched between a silica substrate and an anisotropic polyethylene terephthalate film. Removal of the polymer film and subsequent drying yields a highly birefringent solid layer made of DSCG or DNA, respectively. Substrates with these well-aligned layers can in turn be used to manufacture uniformly aligned samples of a thermotropic liquid crystal. The quality of the align...