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.