A novel strong-fluorescent Tb-containing hydrotalcite-like compound (Tb-HTlc) was prepared using the coprecipitation method. The Tb-HTlc has a special layer structure, in which aluminum(III) was partially substituted by terbium(III) in the hydrotalcite-like layers; acetylacetone and 1,10-phenanthroline were dispersed into the anions among the interlayer region. Tb3+ ions in the layers were coordinated by the acetylacetone and 1,10-phenanthroline through the oxygen and nitrogen atoms. The sample was characterized by X-ray powder diffraction patterns, X-ray photoelectron spectroscopy, fourier transform infrared, thermogravimetry and differential scanning calorimeter (TG-DSC), transmission electron microscopy, and fluorescence spectra, and its properties and structure were determined. The results indicated that the sample exhibited a characteristic green light (545 nm). The fluorescent lifetime and fluorescence quantum yield of Tb-HTlc were measured to be, 1092.88 mu s and 54.07% respectively, higher than those of Tb(III)-acetylacetone-1,10-phenanthroline complex [Tb(acac)(3)phen]. The result of TG-DSC measurement clearly showed the enhanced thermal stability of Tb-HTlc compared with that of MgAl-LDH and Tb(acac)(3)phen. Possessing excellent photoluminescent property and thermal stability, low contents of rare earth ions and ligands, the Tb-HTlc may become one of the novel fluorescent materials with potential application in organic light-emitting diodes.