The nanoscience and nanotechniques have brought with new chance for new applications of some traditional materials, for instance, ceria-based materials, which are of great interest due to their wide applications, in particular, as redox or oxygen storage promoters in the three-way catalysts, catalysts for H(2) production from fuels, and solid state conductors for fuel cells. We highlight here current research activities focused on the controlled synthesis and assembly of ceria-based nanomaterials. We begin with a brief introduction to the urgency for research of ceria-based nanomaterials and our different consideration. Typical synthesis is then discussed with examples of nanosized ceria, ceria-zirconia solid solutions, and doped ceria developed by our group and the others. Controlled synthesis to manipulate the shape, crystal plane, and size is the topic of this article, with approaches elaborated for the assembly of ceria-based materials. Finally, we conclude this article with personal understandings and perspectives on this exciting realm.