Erbium, europium, and cerium co-doped tantalum oxide (Ta2O5:Er, Eu, Ce) thin films were prepared using a simple co-sputtering method, and yellow light emission was observed by the naked eye from a sample annealed at 900 °C for 20 min. The hexagonal Ta2O5 phase is very important, but the hexagonal CeTa7O19 phase should be avoided to obtain strong yellow light emission from Ta2O5:Er, Eu, Ce films. The co-sputtered films can be used as high-refractive-index and yellow-light-emitting materials of autocloned photonic crystals that can be applied to novel light-emission devices, and they will also be used as anti-reflection and down-conversion layers toward high-efficiency silicon solar cells.