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In this paper, thermoluminescence (TL) properties of rare earth Tb3+-doped α-Sr2P2O7 were examined after β-irradiation and photoluminescence (PL) properties of samples were examined for proper excita-tion. All the samples were synthesized by high-tempera-ture combustion method. The X-ray diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy characterization confirms the formation of pure α-phase with crystallized in orthorhombic structure of samples. The PL emission spectra of all samples exhibit charac-teristic green emission peaks of Tb3+ where the peak at 545 nm has the highest emission intensity for Tb3+ con-centration of 5.0 mol%. The TL glow curves of β-irradi-ated Tb3+-doped α-Sr2P2O7 phosphors were recorded at different heating rates of 2, 4, and 6 K?s-1. TL curves of all sample exhibit combination of two peaks: peak at 420 K shifts toward higher temperature, while peak at 525 K remains unaffected with the increase in Tb3+concentration as well as fading effect. The activation energy and kinetic parameters of the samples were eval-uated using thermoluminescence peak shape method.