The persistent luminescent (PSL) phosphors Sr2-x-yMgSi2O7: xEu2+, yDy3+ (x = 0∼0.08, y = 0∼0.08) were synthesized by a solid-state reaction method in a weak reductive atmosphere of 5%-H2/N2. Comprehensive measurements were carried out to study the effects of Eu2+ and Dy3+ doping amount on the crystal phase, photoluminescence (PL), afterglow decay properties, and trap energy levels. The results indicated that the impurity phases decreased and disappeared, and crystalline grains tended to be larger and denser with the doping amount of Eu2+ and Dy3+ increasing. We shed light on the origination of asymmetric PL peak, concentration quenching of Eu2+ ions, time evolution of PSL specture and chromaticity of Eu2+, Dy3+ co-doped phosphors. Based on the deconvolutions of X-ray photoelectron spectroscopy (XPS) spectra and thermoluminescence (TL) spectra, the types and energy depth of traps in these phosphors were systematically studied. According to the data of PL, PLE, and TL, we deduced a schematic diagram of the energy level and discussed the mechanism of PSL of the phosphors. As Dy3+ dopant increases, the Eu2+, Dy3+ co-doped phosphors not only generate more defects of VO•• and VSrʺ, but also introduce DySr• defect with proper trap depth, meanwhile, a thermally assisted tunneling mechanism will gradually dominate during the persistent luminescence, which is responsible for that the phosphor with x = 0.02, y = 0.01 presents the best long afterglow property.