Materials phenomena ranging from the melting or freezing of ice to biomineralization in living organisms, to lubrication and the commercial casting of superalloys, are known to be critically influenced by molecular-scale structure and processes occurring at the interfaces between the crystalline solid and liquid phases. The properties of solid–liquid interfaces have long been a topic of intense interest in materials science, primarily because of their role in governing nucleation, growth, and morphological evolution in crystal growth from the melt or solutions.This issue of the MRS Bulletin provides an overview, highlighting new developments in experiment, theory, and modeling techniques that have led to substantial recent progress in the characterization of the molecular-level structural and thermodynamic properties of solid–liquid interfaces and their consequences for a variety of crystallization phenomena.