A broad class of lyotropic liquid crystals of a non-surfactant nature, the so-called lyotropic chromonic liquid crystals (LCLCs), are alignable with the techniques, in particular, LCLCs can be aligned at a surface as one monomolecular layer as a stack of monomolecular layers. The method for monolayer alignment is based on alternate layer-by-layer adsorption of polyions and dyes from aqueous solutions that have liquid crystalline structure. Using this method, one is able to stack alternate monolayers of dye and polyion while controlling the long-range in-plane orientation of the dye molecules within the plane of each layer. The feature of controlling the alignment of LCLCs enables one to create practical devices from them. For example, alignment of multilayered stacks allows one to use the resulting dried LCLC films in optical devices, for example, as internal polarizers, color filters, optical compensators, band-gap filters, and the like.