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Cerium-doped Gd2SiO5 (GSO) scintillator has good scintillation properties such as high density, intense light output, short decay time, excellent temperature stability, and extremely good energy resolution. In order to apply GSO single-crystal scintillators to a commercial PET, we have tried to increase the size of the GSO single-crystal for increasing production capacity and reducing production cost. To grow the large GSO single-crystal, we have optimized growth conditions and atmosphere in the furnace. We have developed growing technology of large GSO single crystals with a diameter of 100 mm. Thousands of specimens with a size of 4×6×20 mm3 were sampled from each ingot. Uniformity of the light output, energy resolution and decay time in the crystal has been demonstrated for PET application.