Tb3+ is a typical green emitting luminescence center in inorganic compounds. However, the absorption of Tb3+ is very weak in ultraviolet spectral region (from 240 to 400 nm). Ce3+ is often used as a sensitizer to transfer energy to Tb3+. In this paper, Ce3+ and Tb3+ were co-doped into a novel aluminates-borates LaAl2.03B4O10.54. Ce3+ can absorb UV light (from 240 to 340 nm) and transfer absorbed energy to co-doped Tb3+ effectively and bring bright green emission of Tb3+. The crystal structure and fluorescence spectra of phosphors, the efficiency of energy transfer between Ce3+ and Tb3+, decay dynamics, the thermal stability and internal quantum efficiency of luminescence have been investigated in detail. These results indicate that the color tunable LaAl2.03B4O10.54: Ce3+, Tb3+ phosphor is a potential green-emitting material. Especially, analysis about the relationship of the doping concentration of luminescence centers and thermal stability of luminescence points out a feasible way to enhance the thermal stability of luminescence in the future.