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Accurate real-time molecular-level monitoring of the physicochemical properties of species at the solid–liquid interfaces under ambient conditions with good temporal and spatial resolution is an end goal of surface science and analytical chemistry. In situsurface-sensitive Raman techniques, chiefly surface-enhanced Raman spectroscopy (SERS), and more recently shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) have helped to liberate the dependence of surface science on ultrahigh vacuum (UHV) systems. In recent years, owing to the advent of novel surface-sensitive Raman spectroscopic techniques, considerable advancements in understanding have been achieved. Here, our aim is 3-fold: (1) to give a summary of some recent advances of in situRaman spectroscopic techniques, (2) to discuss some of the applications and fields which in situRaman spectroscopic interfacial studies have been applied to date, and (3) to give a perspective of in situRaman spectroscopic techniques for studying solid–liquid interfaces that is accessible to the broader scientific community.