A series of ZnS0.75O0.25:0.1%Ce3+,x%Tb3+ phosphors were prepared by high temperature solid state reaction method. These phosphors exhibited two mixed phases consisting of hexagonal phase ZnS and hexagonal phase ZnO with the average particle size of 13.83 μm and emitted blue-green light. The luminescence mechanism consisted of Zn vacancy defects, the 5d1 → 2F5/2 radiative transitions of Ce3+, the 5D4 → 7F5 and 5D4 → 7F6 radiative transition of Tb3+ induced by the energy transfer of Ce3+ → Tb3+. An equation for the variation of the fluorescence lifetime of ZnS0.75O0.25:0.1%Ce3+,x%Tb3+ phosphors with concentration of Tb3+ fraction was obtained by exponential fitting. The short fluorescence lifetime could be tuned within the range of 113 μs to 550 μs with the increase of Tb3+ concentration, and the color was tunable from blue to blue-green, which is of important application in the field of high-energy particle detection.