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In situ Raman spectroscopy provides access to aqueous interfacial chemistry, adsorbed NO\n                    <jats:sub>x<\/jats:sub>\n                    species, dynamic catalyst phases, and local microenvironments under operating conditions. However, many studies still rely mainly on peak assignment, even though the mechanistic reliability of individual spectral features varies substantially. This Perspective presents a Raman\u2010centered diagnostic framework for nitrate electroreduction. Raman signals are organized into four interfacial readouts: adsorbed nitrate and nitrite species, hydrogenated nitrogen intermediates, catalyst reconstruction, and interfacial water and ion structures. An evidence hierarchy is introduced to assess Raman assignments through isotope labeling, potential\u2010, time\u2010, and space\u2010resolved measurements, multimodal validation, and quantitative correlations with product distributions. 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