Ce3+, Tb3+ co-doped green phosphor Ca2SrAl2O6 was synthesized by solid state method and its excitation and emission spectra were measured and studied. The results showed that the emission spectrum is composed of four groups of narrow bands and the peaks are located at 497, 545, 595 and 623 nm. The strongest emission peak islocated at 545 nm and chromaticity coordinate (x, y) is (0.300 5, 0.500 2) at 4 mol% Ce3+ and Tb3+ doping, which indicate that Ca2SrAl2O6∶Ce3+, Tb3+ was a good green phosphor. The excitation spectrum for 545 nm was in the region of 320-400 nm, which indicated that this phosphor could be effectively excited by UVLED. Duo to the overlap of the Ce3+ emission bands and the Tb3+ excitation bands, the energy transfer between Ce3+ and Tb3+ is expected to be very efficient. The emission intensity of co-doped Ca2SrAl2O6 phosphor was stronger than that of Tb3+ doped phosphor. The luminescence intensity reached the maximum when the concentration of Ce3+ and Tb3+ was 4 mol%.