We report the use of an efficient hydrothermal method to synthesize superparamagnetic and red luminescent bifunctional Fe3O4@Mn2+-doped NaYF4:Yb/Er nanoparticles (NPs) with core@shell structures via a seed-growth procedure. Oleic acid coated Fe3O4 (OA-Fe3O4) NPs were initially synthesized using a coprecipitation method. The as-synthesized OA-Fe3O4 NPs were then used as seeds, on which the red upconversion luminescent shell (Mn2+-doped NaYF4:Yb/Er) was formed. Furthermore, hydrophobic to hydrophilic surface modification of the Fe3O4@Mn2+-doped NaYF4:Yb/Er NPs was achieved via a ligand exchange method where oleic acid was displaced by a PEG phosphate ligand [PEG = poly(ethylene glycol)]. These materials were characterized by means of transmission electron microscopy (TEM), X-ray diffraction (XRD), photoluminescence (PL) spectroscopy, and vibrating sample magnetometry (VSM). The Fe3O4 cores were uniformly coated with a Mn2+-doped NaYF4:Yb/Er shell, and the bifunctional Fe3O4@Mn2+-doped NaYF4:Yb/Er NPs were monodispersed. Furthermore, the Fe3O4@Mn2+-doped NaYF4:Yb/Er NPs exhibited a saturated magnetization value of 6.2 emu/g and emitted red luminescence under a 980 nm laser. The obtained bifunctional Fe3O4@Mn2+-doped NaYF4:Yb/Er NPs may find potential applications in drug targeting, bioseparation, and diagnostic analysis. The synthetic method may be employed for the preparation of other bifunctional nanomaterials. (C) 2016 Elsevier B.V. All rights reserved.