Luminescent-magnetic bifunctional NaGdF4:Eu3+ nanofibers were fabricated through the bond of electrospinning followed by calcination with fluorination technology for the first time. The structure, morphologies, luminescence, and magnetism of nanofibers have been characterized using various techniques. X-ray diffraction measurement indicates that NaGdF4:Eu3+ nanofibers are hexagonal phase. Scanning electron microscope measurement shows that the mean diameters of electrospinning-made polyvinyl pyrrolidone/[NaNO3+Gd(NO3)(3)+Eu(NO3)(3)] composite nanofibers and NaGdF4:Eu3+ nanofibers are, respectively, 428 +/- 4 and 231 +/- 4 nm under the confidence level of 95%. Under 274-nm ultraviolet light excitation, NaGdF4:Eu3+ nanofibers exhibit characteristic (D3,2,1,0FJ)-D-5-F-7 emissions of Eu3+ and the tendency of color tones of samples varies from blue, cold white, warm white to red via varying Eu3+ content. In addition, samples exhibit paramagnetic features and the magnetic properties of NaGdF4:Eu3+ nanofibers are tailorable by modulating the doping concentration of Eu3+. More importantly, the color-tailorable luminescence and paramagnetic properties are simultaneously realized in single-phase NaGdF4:Eu3+ nanofibers, which ideally suit to apply in many fields such as lighting and color displays, bioimaging, and magnetic resonance imaging. This design conception and construction strategy may provide some new guidance for synthesizing other rare-earth fluorides nanomaterials of multifarious morphologies.