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This study reports in situ observations of the formation of the δ′-ZrO phase, occurring during the annealing of transmission electron microscopy (TEM) thin foils of both pure Zr and a Zr–Sn–Nb–Mo alloy at 973 K in a transmission electron microsope. The lattice parameters of δ′-ZrO were measured and determined to be similar to those of the ω-Zr phase. The orientation relationship between the δ′-ZrO and α-Zr phases has been identified as either and or and depending on the orientation of the α grain relative to the TEM thin-foil normal. The nucleation and growth of δ′-ZrO were dynamically observed. This study suggests a new and convenient way to study oxidation mechanisms in Zr alloys and provides a deeper understanding of the properties of the newly reported δ′-ZrO. Since δ′-ZrO has a Zr sublattice which is identical to that of ω-Zr, the orientation relationships between the α and δ′-ZrO phases may also shed light on the orientation relations existing between α- and ω-Zr, and hence α- and ω-Ti.