Solid-state lighting devices, thermoluminescence dosimeters, and photoluminescence dosimeters are commonly utilized in radiation environment monitoring. The development of new thermoluminescence and photoluminescence materials has become a primary focus in radiation dosimetry research, as the performance of dosimeters is directly tied to the materials used. As a result, the study and development of innovative thermoluminescence and photoluminescence materials have gained significant attention in recent years. In this study, the high-temperature solid-state method was employed to synthesize Gd2Si2O7 doped with varying amounts of Sm3+. To investigate the crystal structure, morphology, thermoluminescence (TL), and photoluminescence (PL) properties of Sm3+-doped Gd2Si2O7, a range of techniques, including X-ray diffraction (XRD), scanning electron microscopy (SEM), TL, and PL, were applied. The results revealed that the highest TL intensity occurred in Gd2Si2O7 doped with 0.7 mol% Sm3+, while the material also exhibited superior PL performance. Overall, Gd2Si2O7 doped with 0.7 mol% Sm3+ shows significant promise for thermoluminescence dosimetry applications due to its outstanding TL properties. Additionally, the photoluminescence of the Sm3+-doped Gd2Si2O7 was analyzed