A series of BaGdF5:Eu3+/Tb3+ orange-green-yellow-white emitting nanophosphors (NPs) were successfully synthesized via hydrothermal method without assistance of any surfactant, catalyst, or template. The nanocrystals are in sphere-like morphology with an average size of approximately 46nm. The quenching concentrations of Eu3+ and Tb3+ single doped BaGdF5 phosphors are 5.5% and 15%, respectively. The tunable color tone can be obtained in Eu3+ and Tb3+ co-doped BaGdF5 phosphors, the strong orange-white and green-yellow emissions can be seen in BaGdF5:5.5%Eu3+, y%Tb3+ and BaGdF5:3.5%Tb3+, x%Eu3+ phosphors, especially. More significantly, we realize the more standard white emission with a CIE chromaticity diagram point at (0.317, 0.321) and a lower correlated color temperature of 6979K in the BaGdF5: 5.5%Eu3+, 4.5%Tb3+ sample. In addition, the energy transfer phenomenon from Tb3+ to Eu3+ ions is clearly observed in Tb3+, Eu3+ co-doped BaGdF5 phosphors and the energy transfer efficiency can reach a maximum of 75%. Moreover, the as-prepared samples exhibit paramagnetic properties at room temperature. This type of multifunctional multicolor emitting nanophosphor has promising applications in the fields of full-color displays, biomedical science, MRI, and so on.