A series of CaSrSiO4 nanophosphors with different Tb3+-doped concentrations have been prepared by high-temperature solid-state reaction method. SEM image shows that the powder particles show a shape of ball and a diameter of about 30~50nm. XRD pattern of the samples doped Tb3+ ions is basically consistent with that of CaSrSiO4 matrix, indicating that Tb3+ dopant has little influence on the crystal structure of CaSrSiO4 powder. Under the 285nm excitation, the intense ultraviolet, blue and green PL spectra are observed and the optimum Tb3+-doped concentration is 0.7%. Finally, the CaSrSiO4∶0.3Tb3+ phosphor is annealed by CO2 laser and its spectral intensity is enhanced by more than 50%. At the same time, the effect of annealing process parameters on PL characteristics of CaSrSiO4∶Tb3+ phosphor is discussed.