Fe3O4/PVP//Tb(BA)(3)phen/PVP magnetic-photoluminescent bifunctional bistrand aligned composite nanofibers bundles based on Fe3O4 nanoparticles (NPs) and terbium complex Tb(BA)(3)phen (BA = benzoic acid) were fabricated by employing a parallel axial electrospinning setup and were characterized by X-ray diffraction, field-emission scanning electron microscopy (FESEM), energy dispersive spectroscopy (EDS), transmission electron microscopy, fluorescence spectroscopy, and vibrating sample magnetometer. It is found that Fe3O4 NPs were only dispersed into one strand of the bistrand aligned composite nanofibers bundles, but no nanoparticles in the other strand. And the average diameter of the individual strand fiber was 200 +/- A 25 nm. The bistrand aligned composite nanofibers bundles exhibit strong green emissions under the excitation of 275 nm ultraviolet light, and the (5) D (4) -> (7) F (5) hypersensitive transition at 545 nm was the predominant emission peak of Tb3+ ions. The newly obtained bifunctional nanofibers bundles exhibit excellent magnetism and high fluorescence intensity and are expected to apply in biology cell separation, magnetic resonance imaging, drug deliver, and fluorescence immunoassays/imaging.