Zn2Ga2.98Ge0.75-xSixO4:Cr3+0.02 (ZGGSO:Cr3+) persistent luminescent nanoparticles were synthesized through a hydrothermal method along with a subsequent vacuum annealing. For these nanoparticles, it is found that NIR emissions peaked at 712 and 697 nm, originating from the 4T2-and 2E-4A2transitions of Cr3+, respectively, appear and Si4+ ions simultaneously substitute for the surface and interior Ge4+ ions. In particular, Si doping leads to the increased average particle size, the decreased crystal field strength and the tunable changes in trap depths and the energy transfer between Cr3+ and deep traps. In the case of a small amount of Si, the afterglow intensity is enhanced compared to the undoped sample due to Si doping leading to the facilitated thermal activation and tunneling processes. As the amount of dopant increases to 0.10, although the afterglow intensity is almost the same with that of the undoped sample, the dispersibility of the nanoparticles in aqueous solution is significantly enhanced. These conclusions indicate that ZGGSO:Cr3+ nanoparticles have potential in in vivo biological imaging.