Magnetic nanocomposite materials consisting of 5.5 wt% Fe-Co alloy nanoparticles in a silica aerogel matrix, with compositions FexCo1−x of x = 0.50 and 0.67, have been synthesized by the sol-gel method. The high-resolution transmission electron microscopy images show nanoparticles consisting of single crystal grains of body-centered cubic Fe-Co alloy, with typical crystal grain diameters of approximately 4 and 7 nm for Fe0.5Co0.5 and Fe0.67Co0.33 samples, respectively. The energy dispersive X-ray (EDX) spectra summed over areas of the samples gave compositions FexCo1−x with x = 0.48 ± 0.06 and 0.68 ± 0.05. The EDX spectra obtained with the 1.5 nm probe positioned at the centers of ∼20 nanoparticles gave slightly lower concentrations of Fe, with means of ⟨x⟩ = 0.43 ± 0.01 and ⟨x⟩ = 0.64 ± 0.02, respectively. The Fe0.5Co0.5 sample was studied using electron energy loss spectroscopy (EELS), and EELS spectra summed over whole nanoparticles gave x = 0.47 ± 0.06. The EELS spectra from analysis profiles of nanoparticles show a distribution of Fe and Co that is homogeneous, i.e., x = 0.5, within a precision of at best ±0.05 in x and ±0.4 nm in position. The present microscopy results have not shown the presence of a thin layer of iron oxide, but this might be at the limit of detectability of the methods.