The synthesis of FeCo alloys as highly magnetic nanoparticles has been valuable, as far as applications for magnetic nanoparticles are concerned. However, recently, a field of magnetoplasmonics in which magnetic nanoparticles such as the FeCo alloys doped with plasmonic materials such as Au and Ag to create a hybrid nanostructure with both properties has emerged. These magnetoplasmonic metamaterials have greatly enhanced the limit of detection of analytes in spectroscopic methods, as well as providing a more widely applicable nanoparticle to broaden the use of FeCo alloys even further. Herein, we discuss the synthesis of high-yield and fairly monodisperse spherical FeCo and Au-doped FeCo (Au@FeCo) with varying compositions of Au synthesized via the thermal decomposition of iron pentacarbonyl (Fe(CO) 5 ) and dicobalt octacarbonyl (Co 2 (CO) 8 ), followed by the addition of Au atoms using triphenylphosphine gold(I) chloride ((Ph 3 P)AuCl) via both coprecipitation and by delayed addition methods. The products were separated using a hand-held magnet, and then characterized via ultraviolet−visible light (UV-vis), scanning electron microscopy coupled with energy-dispersive X-ray analysis (SEM-EDX), high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), flame atomic absorption spectrometry (F-AAS), and magnetization measurements. Optical studies revealed a plasmonic peak at 550 nm in the Au@FeCo nanoparticles that had a gold content (%Au) of >2% (by weight), determined using F-AAS. Colocation of the Fe, Co, and Au were demonstrated through EDX analysis. Location of the Au atoms in the core were seen through high-resolution bright-field imaging. To understand the use of these nanoparticles for potential application in therapeutics and/or electronics, resistance measurements were performed to assess power loss as a function of frequency. We also achieved magnetization values as high as 150 emu/g and as low as 50 emu/g for gold-loaded samples based on % Au by weight. This paves the way to continue to develop magneto-plasmonic structures chemically using these synthesis strategies.