The ability to manipulate the multicolor luminescence will greatly enhance the scope of their applications, ranging from infrared solar cells to volumetric multiplexed bioimaging. Tuning from yellow to red emission was successfully achieved in Eu/Er:LiNbO3 under ultraviolet (UV) and blue excitation. The excitation spectra of Eu/Er:LiNbO3 monitored at 590 nm/618 nm/626 nm were studied. The CIE 1931 color coordinates showed that the emissions fell within the yellow and red region, respectively, under 376 nm and 397 nm excitation. The color coordinates shifted from yellow toward red region upon diode laser excitation of 476 nm.