Catalysis is a complex multidisciplinary science that enables efficient performance in energy, automotive, chemical and pharmaceutical industries; most chemical reactions are catalyzed and it is a science that cannot be understood without spectroscopy. Spectroscopy is the enabling tool for knowledge-based design of highly efficient and stable catalysts. This review presents the progress of operando Raman spectroscopy during reaction and temperature-programmed treatments for heterogeneous catalysts (solid-gas and solid-liquid), with particular emphasis on the combination with other techniques, by extending it to space-resolved analyses and as a tool for mechanism investigation and monitoring in the liquid phase. Operando techniques are a key tool to understand catalysis and for monitoring and controlling catalytic processes. We summarize the most relevant research lines where Raman spectroscopy is applied in catalysis, challenges, hurdles and opportunities. This review outlines the versatility of Raman spectroscopy, for real-time analyses, in situ variable-programmed investigations and reaction studies. Spectroscopic information can be enhanced in a quantitative or qualitative manner, i.e., by using high-throughput Raman setups or by combining several spectroscopic techniques in a sample, respectively. This compilation outlines the posibilities of signal enhancement by resonance or SERS, and expanding it to mapping. We also comment developments for Raman imaging of profiles during catalyst synthesis and during reaction. Finally, this review summarizes the progress made in the liquid phase, to study catalyst synthesis, to monitor and investigate reaction mechanism and progress. The simultaneous combination of Raman with other complementary techniques is presented for these three lines of development. The current scenario presents an extraordinary perspective on opportunities for future developments.