A review. CeO2 is widely used and investigated as an oxide catalyst or support due to its unique redox property of oxygen storage and release. In this paper, the different opportunities offered by Raman spectroscopy for advanced characterization of ceria-based catalysts are reviewed: spectral modifications induced by nanocrystallinity, defects, doping and reduction, identification of supported molecular species, isolated atoms and nanoclusters, characterization of surface modes, hydroxyl groups, reaction intermediates such as peroxo and superoxo species. Finally, in situ/operando studies for environmental catalysis are summarized illustrating Raman spectroscopy as a powerful tool to characterize ceria-based catalysts.