A lanthanum pyrosilicate (La2Si2O7, LaPS) single crystal is successfully grown with a Ce-doped concentration of 0.5 to 20.0% as well as undoped LaPS for reference. The photoluminescence emission map of Ce-doped LaPS has broad emission at 360–410 nm from Ce3+ 5d-4f transition, with a decay time of 20–24 ns. In the scintillation properties, Ce-doped LaPS presents the scintillation peak at 390 nm under X-ray excitation, with the decay time constant at 26–31 ns plus another decay constant caused by the emission from host material at 250–600 ns. The afterglow level at 20 ms after X-ray irradiation is around 30–56 ppm. In the 662 keV γ-ray pulse height spectra, 1.0% Ce-doped LaPS shows a clear photoabsorption peak, with a scintillation light yield of 5400 ph MeV−1. The relationship between γ-ray energy and the photoabsorption peak channel (linearity) is also covered in this study.