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The atomic-scale study of solid-solid interfaces in complex multi- phase multi-component systems is a challenging but important endeavor. This article highlights the coupling of recently developed advanced characterization techniques, such as high resolution scanning transmission electron microscopy (HRSTEM), carried out in an aberration-corrected microscope, and 3D atom probe (3DAP) tomography, to address the structural and compositional transition at the atomic scale across solid-solid interfaces, such as the gamma/gamma interface in Ni-base superalloys and the alpha/beta interface in titanium alloys. Possible implications of such investigations of the interface on the understanding of physical and mechanical properties are discussed.