Molecular self-assembly is the most important strategy for the developmentofchiralaggregates andchiralfunctionalmaterials. In this study, we rationally designed and synthesizedchiralfluorescent heteroclusters that were self-assembled into microscalecubosomeswith a three-dimensional (3D)bicontinuouscubicphase nanostructure. Thecubosomesexhibitedchirality, indicating thatchiralityis transferred from the molecules to the 3D nanostructure. Therefore, we confirmed the formationofachiralbicontinuouscubicphase nanostructure for the first time. We also showed that thischiralityoriginates from the continuous change in the saddle-splay distortionofthe molecules within the curved bilayer. At the same time, transparent filmsofchiralcompositeswere prepared by mixing thechiralcubosomeswith an epoxy resin and then curing the mixture. Therefore, we demonstrated an effective method for preparingchiralcomposites. (C) 2021 Published by Elsevier B.V. on behalfofChinese Chemical Society and InstituteofMateria Medica, Chinese AcademyofMedical Sciences.