Ta2O5–xEr2O3 (TE) films were produced by a sol-gel method and a dip-coating technique with heat treatment at 600–1000 °C. Their powders were also prepared from the same sol. The Er3+ fluorescence property of the TE films containing various contents of Er3+ was measured as a function of the heat-treatment temperature. In crystallized films, the Er3+ fluorescence was observed because water-related residues (Ta–OH and H2O) and carbon-related residues (–CH3, –CH2–, –(C ⁼ O)–, and C≡C–H) were removed from the films. It is shown from infrared absorption spectroscopy that Ta–O− and Ta ⁼ O structures dissolve the Er3+ ions selectively and play a role in dispersing the Er3+. The strongest Er3+ fluorescence is observed in the TE film with 2 mol% of Er2O3 because of its highest ability to disperse the Er3+ ions.