Electrochemical energy conversion technologies offer sustainable routes for the production of fuels and value-added chemicals; however, achieving efficient, selective, and durable electrocatalytic systems requires a fundamental understanding of the dynamic processes occurring at the electrode–electrolyte interface under realistic operating conditions (>1Acm-2 ). In this seminar, I will highlight recent advances in integrating catalyst design with operando spectroscopic investigations to uncover the dynamic evolution of electrochemical interfaces during electrocatalytic reactions. Beginning with the rational design of electrocatalysts for water electrolysis and mechanistic investigations into the role of cation concentration, electrolyte environment, and interfacial water in electrocatalytic reactions, I will then describe the development of an operando Raman spectroscopy platform capable of probing electrochemical interfaces at industrially relevant current densities (up to 1 A cm-2 ). Particular emphasis will be placed on understanding the dynamic restructuring of interfacial water, the evolution of surface-bound reaction intermediates, and their interplay in governing electrocatalytic performance. Furthermore, the application of two-dimensional correlation spectroscopy enables the sequential evolution of interfacial species to be resolved, providing mechanistic insights that are difficult to obtain using conventional spectroscopic approaches. Finally, I will discuss future opportunities for extending operando Raman spectroscopy to increasingly complex electrochemical systems. Advancing these methodologies will enable a deeper understanding of electrochemical interfaces under practical operating conditions and open new avenues for the development of next-generation electrocatalytic technologies for sustainable energy conversion.