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Cerium-doped gadolinium pyrosilicate single crystals Ce:Gd2Si2O7 (Ce:GPS) with various Ce concentrations of 2.5-30 mol% with respect to the total rare-earth sites were prepared by the floating zone method. Their scintillation performances were investigated under irradiation of gamma rays of 137Cs. The Ce concentration dependence of scintillation characteristics and high-performance scintillation characteristics were obtained: 3-6 times greater light output than that of BGO single crystals, rapid decay, and good energy resolutions of 5.1-8.4%. Furthermore, X-ray diffraction patterns of Ce:GPS revealed Ce concentration dependence of the crystal structure of Ce:GPS.