Samples of natural andalusite (Al2SiO5) crystal have been investigated in terms of thermoluminescence (TL) and electron paramagnetic resonance (EPR) measurements. The TL glow curves of samples previously annealed at 600 °C for 30 min and subsequently gamma-irradiated gave rise to four glow peaks at 150, 210, 280 and 350 °C. The EPR spectra of natural samples heat-treated at 600 °C for 30 min show signals at g=5.94 and 2.014 that do not change after gamma irradiation and thermal treatments. However, it was observed that the appearance of a paramagnetic center at g=1.882 for the samples annealed at 600 °C for 30 min followed gamma irradiation. This line was attributed to Ti3 centers. The EPR signals observed at g=5.94 and 2.014 are due to Fe3. Correlations between EPR and TL results of these crystals show that the EPR line at g=1.882 and the TL peak at 280 °C can be attributed to the same defect center. © 2011 Elsevier B.V. All rights reserved.