A method of making a multilayered chromonic structure comprises (a) preparing a first aqueous mixture comprising (i) a first continuous water-soluble polymer phase and (ii) a first discontinuous chromonic phase comprising a chromonic material, to form chromonic nanoparticles;(b) non-covalently crosslinking the resulting chromonic nanoparticles with a multivalent cation salt; (c) dispersing the resulting crosslinked chromonic nanoparticles in a composition comprising a chromonic material to form a chromonic nanoparticle dispersion; and (d) preparing a second aqueous mixture comprising (i) a second discontinuous chromonic phase comprising the chromonic nanoparticle dispersion and (ii) a second continuous water-soluble polymer phase, to encapsulate the chromonic nanoparticles; wherein at least one of the first discontinuous chromonic phase and the second discontinuous chromonic phase further comprises a guest compound.