Luminescent-magnetic bifunctional NaGdF4:Dy3+,Eu3+ nanofibers have been successfully fabricated via the combination of electrospinning followed by calcination with fluorination technique for the first time. The structure, morphologies, luminescence, and magnetic properties of the synthesized nanofibers have been characterized by a variety of techniques. X-ray diffraction (XRD) analysis shows that as-prepared NaGdF4:Dy3+,Eu3+ nanofibers are pure hexagonal structure. Scanning electron microscope (SEM) observations indicate that directly electrospinning-made PVP/[NaNO3 + Gd(NO3)(3) + Dy(NO3)(3) + Eu(NO3)(3)] composite nanofibers have smooth surfaces, good dispersion and uniform size, and the surfaces of NaGdF4: Dy3+,Eu3+ nanofibers become rough after calcination and fluorination process. The diameters of composite nanofibers and NaGdF4:Dy3+,Eu3+ nanofibers are respectively 400.19 +/- 48.06 nm and 245.90 +/- 52.10 nm. NaGdF4:Dy3+,Eu3+ nanofibers exhibit predominant visible emission under 274 nm ultraviolet light excitation and the trend of their color tones changes from blue, cold white, warm white to red by adjusting the molar concentration of Eu3+. In addition, all of the samples exhibit paramagnetic features and the magnetic properties of NaGdF4:Dy3+,Eu3+ nanofibers are tunable by changing the species and doping concentration of RE3+ ions. More importantly, the tunable multicolor luminescence and paramagnetic properties are simultaneously realized in single-phase NaGdF4:Dy3+,Eu3+ nanofibers, which ideally suit to apply in many fields such as solid-state lasers, lighting and displays, magnetic resonance imaging. This design conception and construction strategy developed in this work may provide some new guidance for the synthesis of other rare earth fluorides nanostructures with various morphologies. (C) 2016 Elsevier B.V. All rights reserved.