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Materials in single crystal form are often sought after because the absence of grain boundaries can result in unique properties relative to the polycrystal, but producing these materials is typically a slow and complex process. In this work, pseudo single crystals of the pseudobrookite compound CoTi₂O₅were synthesized by solid‐state reaction from a duplex grain mixture of CoTiO₃and TiO₂. The size of the crystallites was >250 µm. The transformation and subsequent microstructural evolution of the CoTi₂O₅was studied by scanning electron microscopy (SEM), electron backscatter diffraction (EBSD), transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), and X‐ray diffraction (XRD). A novel growth mechanism was identified whereby a single crystal CoTi₂O₅front advances simultaneously along multiple CoTiO₃/TiO₂diphasic boundaries. The single crystal domains were composed of subgrains approximately 5 µm in diameter; differences in the subgrain size and misorientation were related to the growth mechanism and the initial grain size of the duplex CoTiO₃–TiO₂mixture. CoTi₂O₅is a little characterized compound, and this study represents the most significant microstructural study of CoTi₂O₅to date. The findings may be applied to similar pseudobrookite compounds such as MgTi₂O₅and Al₂TiO₅.