As the widespread application of white light-emitting diodes (WLEDs) in lighting field and liquid crystal display (LCD) backlight, the development of phosphors toward multifunctional applications is considered to be an inevitable tendency. In this work, multi-color light emissions have been realized in Eu2+ and Mn2+-activated magnetoplumbite-type GdMgAl11O19 (GMAO) along with adjustable photoluminescence properties. Significantly, a promising narrow-band green light emission can be achieved by Mn2+-activated GMAO with the full width at half maximum (FWHM) of 27 nm, and such narrow emission band makes the as-prepared WLED device reach 121 % of National Television Standards Committee (NTSC), which can act as an ideal LCD backlight. On the other hand, the broad cyan light can be achieved in Eu2+-activated GMAO. Moreover, multi-color light emissions have been realized in Eu2+ and Mn2+ co-doped GMAO, and the energy transfer from Eu2+ to Mn2+ ions was established. Benefitting from the broad band cyan light emission of Eu2+ ion, a promising WLED device with high color rendering index (CRI) of 90 has been fabricated by using Eu2+ and Mn2+ co-doped sample. The result indicates the multifunctional applications of the GMAO modulated by Eu2+ and Mn2+ activators.