In recent years, it is heartening to witness that carbon quantum dots (CQDs), a rising star in the family of carbon nanomaterials, have displayed tremendous applications in bioimaging, biosensing, drug delivery, optoelectronics, photovoltaics and photocatalysis. However, the investigations toward self-assembly of CQDs are still in their infancy. The participation of CQDs can bring additional functions to supramolecular self-assemblies, with photoluminescent property as the most exciting aspect. Here, we introduce CQDs into two types of classic colloidal systems containing low molecular weight surfactant and gelator to construct fluorescent vesicles and chiral hydrogels. The CQD-based vesicles were constructed through electrostatic interaction between the positively charged CQDs with peripherally substituted imidazolium cations and a negatively-charged biosurfactant, i.e., sodium deoxycholate (NaDC). The chiral hydrogels were prepared by increasing the concentration of NaDC and addition of a tripeptide (glutathione, GSH). It was found that both the hydrogels and corresponding xerogels are highly photoluminescent. A solid sensing system was prepared by coating a uniform layer of the hydrogel onto the silica gel plates by doctor blade technique followed by air-drying, which was then utilized to semiquantitatively detect Cu2+ in aqueous solutions.