Display omitted •Structural relaxation controls technological utility of glasses and glass-ceramics.•NMR studies of relaxation in inorganic glass-forming liquids are reviewed.•Connection between atomic dynamics and liquid-to-glass transition is established. Dynamical NMR spectroscopy provides unique mechanistic understanding of the transport and relaxation processes in glass-forming liquids over timescales typically ranging from ~10−9 s to ~102 s, and thus has been used extensively in the past to study the dynamical behavior of polymeric and organic glass-forming liquids. However, reports in the literature of similar studies on inorganic glass-forming liquids have remained somewhat limited due to the experimental challenges. In this contribution we present a review of the high-temperature NMR spectroscopic studies of atomic and molecular dynamics in a wide variety of inorganic glass-forming liquids including oxides, halides and chalcogenides as well as select ionic liquids and molten salts. The significance of these dynamical processes in understanding the nature of the liquid-to-glass transition and their connection with the macroscopic transport properties of these liquids are discussed.