Three-dimensional flowerlike europium-doped lanthanide molybdate [La
2(MoO
4)
3:Eu] microarchitectures thatexhibit efficient photoluminescence have been successfully synthesized via a facile hydrothermal process inthe presence of the surfactant bis(2-ethylhexyl)sulfosuccinate (AOT). The La
2(MoO
4)
3:Eu microspheres arewell dispersed, have a uniform diameter of about 3
m, and are composed of nanoflakes of about 30-nmthickness that connect to each other by both edge-to-edge and edge-to-flat-surface conjunctions with fewsurface-to-surface attachments. The surfactant NaAOT was found to play a crucial role in achieving the gooddispersibility and uniform morphology of the final product, as compared to the same material but synthesizedwithout the surfactant. The UV absorption results illustrate that there is a 20-nm blue shift of CT band relativeto bulk materials, which can be attributed to the quantum size effects of the nanoflakes. These La
2(MoO
4)
3:Eu microspheres show efficient photoluminescence that is associated with the well-crystallized structures ofthe microarchitectures.