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The titanium barium glass microspheres doped with Er2O3 were designed and prepared. The components of the glass sample were 25TiO2-27BaCO3-8Ba(NO3)2-5ZnO2-10CaCO3-5H3BO3-10SiO2-7water glass-3Er2O3 (%, mass fraction). The emission spectra of titanium barium glass matrix and the titanium barium glass microsphere under 514 nm excitation were measured with micro-Raman spectrometer. Whispering gallery modes in the emission spectra from a 31 μm glass microsphere were observed. Many regularly spaced, sharp peaks appeared in the emission spectra of the Er2O3-doped glass microsphere. The wavelength separation between the two adjacent peaks is 1.92 nm for the 31 μm microsphere. According to the Lorenz-Mie formula, the calculated value of the wavelength separation between the two adjacent peaks is 1.95 nm. The observed resonances could be assigned by using the well-known Lorenz-Mie formula.