Solidification processing offers the first opportunity to control microstructure, properties, and performance in metallic alloy components. Until recently, microstructural evaluations were limited to post-solidification characterization by destructive methods. We review the development of time-resolved, in situ imaging techniques capable of capturing solid–liquid interfacial evolution in metallic alloys with high spatial and temporal resolution under diverse solidification conditions relevant for applications ranging from conventional directional solidification, crystal growth, and casting, to welding and additive manufacturing. These experiments enable direct visualization of transient behaviors that would otherwise remain unknown, uniquely providing insights into the physics that impact microstructure and defect development, and strategies for microstructural control and defect mitigation. Understanding microstructural evolution and the characteristics that form under various solidification conditions is essential for the development of multiscale, experimentally informed predictive modeling. This is highlighted by solidification simulations that utilize in situ measurements of solidification dynamics from state-of-the-art experimental techniques.