A unique class of impurity-based quasi-liquid films has been widely observed at free surfaces, grain boundaries (GBs), and hetero-phase interfaces in ceramic and metallic materials (Figure 1). These nanometer-thick interfacial films can be alternatively understood to be: (a) quasi-liquid layers that adopt an “equilibrium” thickness in response to a balance of attractive and repulsive interfacial forces (in a high-temperature colloidal theory) or (b) multilayer adsorbates with thickness and average composition set by bulk dopant activities [1–2]. In several model binary systems, such quasi-liquid, interfacial films are found to be thermodynamically stable well below the bulk solidus lines, provoking analogies to the simpler interfacial phenomena of premelting in unary systems [3] and prewetting in binary de-mixed liquids [4]. These interfacial films exhibit structures and compositions that are neither observed nor stable as bulk phases, as well as transport, mechanical, and physical properties that are markedly different from bulk phases.