In the present work, nanostructured aluminum titanate (Al2TiO5 or AT) was synthesized by the sol-gel method and potential effects of mechanical strain on its phase analysis, morphology, and thermal stability were investigated in some details for the first time, because the thermal instability of AT is beneficial to the fabrication of in-situ aluminum matrix composites. To characterize the particle distribution, microstructure and thermal durability of AT after the strain induction, field-emission scanning electron microscope (FE-SEM), differential scanning calorimetry (DSC), and x-ray diffraction analysis (XRD) were utilized. The experimental results showed that a 3-h ball milling process could impose 0.32% lattice strain on this powdery ceramic and contribute to its destabilization. This strain is able to considerably change the AT morphology from particulate to fibrous one, but it does not affect its phase analysis. More importantly, the induced strain is able to noticeably accelerate the dissociation rate of AT and reduce its decomposition temperature from 950 to 250 degrees C. Moreover, this one-step decomposition occurs in three distinct steps after the mechanical strain. It means that AT bears a significant strain sensitivity.