Nanosheets, which are ultrathin inorganic crystals, have the potential to exhibit unique surface states and quantum effects. These nanosheets can be further manipulated to form lamellar structures for the fabrication of advanced hybrid nanomaterials. Here we report that conventionally nonluminescent ceria yields intense UV photoluminescence with an internal quantum yield (QY) of 59% when self-organized into a nanosheet lamellar architecture with dodecyl sulfate (DS) bilayers. The origin of luminescence exist at the organic/inorganic interfaces, where surface Ce(3+) ions of ceria nanosheet layers graft with DS anions to activate radiative 5d → 4f transition.