High refractive index composites of iron sulfides and poly(ethylene oxide) (PEO) have been prepared by co-precipitation from aqueous solution. Several reaction parameters were varied: inorganic reactants, reactant ratios, reaction temperatures, and reaction times. Selected samples were characterized with organic microelemental analysis, x-ray fluorescence spectroscopy, x-ray diffraction, DSC, and TEM. The nanocomposites with the highest refractive indices have been prepared using PEO, Mohr's salt, and H2S or NaHS. The analyses indicate that the iron sulfides in these materials consist of finely dispersed mackinawite and greigite (“amorphous” FeS) and, partially, also pyrite. The refractive indexes of the resulting composites are clearly above 2 at 632.8 and 1295 nm and can assume values between 2.5 and 2.8.