This chapter focuses on the application of Raman spectroscopy for characterizing catalytic materials and for the investigation of the bulk and surface chemistry occurring during catalyst preparation and operation; a general theoretical background and description of equipment for Raman experimentation is also presented. Over the past decades, Raman spectroscopy has increasingly been applied for characterization of all types of catalytic materials: bulk and supported metals, bulk mixed metal oxides, supported metal oxides, bulk and supported metal sulfides, zeolites and molecular sieves, heteropolyoxo anions, and clays. Raman is also used to study chemisorption and, in recent years, Raman has been increasingly applied under in situ conditions. There is an increasingly important strong driving force leading research toward the study of catalysts under reaction conditions. The last few years exhibit an increasing number of Raman studies during relevant reaction conditions (operando methodology). This momentum in reaction and operando Raman spectroscopy advances a new revolution in catalysis science that is poised to afford accurate molecular understanding of catalytic structure–activity/selectivity relationships.