In this work, bifunctional nanoparticles (NPs) capable of emitting near infrared (NIR) fluorescence and generating superparamagnetism under an external magnetic field were prepared by combination of 'click' reaction and surface-initiated activators generated by electron transfer for atom transfer radical polymerization (AGET ATRP) of water-soluble poly(ethylene glycol) monomethyl ether methacrylate (PEGMA) and glycidyl methacrylate (GMA) using biocompatible iron as the catalyst on the surface of silica-coated iron oxide (Fe3O4@SiO2) NPs. The nanosized Fe3O4@SiO2@PPEGMA-co-PGMA@N3 was prepared through AGET ATRP and alkynyl bearing NIR dye was also prepared; afterwards they were integrated together by 'click' reaction. The different stages of surface modification were approved by employing different characterization techniques such as TEM, XRD, XPS, VSM and FT-IR, and the properties of the final NPs were thoroughly studied. Their suitability as dual model imaging agents for magnetic resonance (MR) and fluorescence imaging was investigated, indicating them to be a competitive candidate for imaging contrast agents.