The large negative temperature coefficient of resonant frequency ( τ f ) of Al2O3 is a problem for applicable microwave/millimeter wave dielectrics. A Previous study reported that the τ f was improved by sintering with TiO2 and then annealing, where the annealing decompose the secondary phase of Al2TiO5. This study investigated the hold time of annealing. The Quality factor (Qf ) value decreased when the sample was annealed at 1100°C for 2hrs. While Al2TiO5 was not detected by X-ray powder diffraction, it was located around TiO2 by scanning transmission electron microscopy equipped with energy dispersive X-ray spectroscopy. It should be considered that the degradation of the Qf was caused by the existence of noncrystalline Al2TiO5 and new boundaries between noncrystalline Al2TiO5 and TiO2.