A method for synthesizing iron-containing nanocomposite based on fibroporous polytetrafluoroethylene (PTFE) is described. Fibroporous PTFE obtained under the radiation of a CO2 laser on block PTFE is modified in supercritical carbon dioxide (sc CO2) to form micro- and nanoporous structures. Porous fluoropolymer is treated with a solution of bis(toluene)iron(0) obtained by metal-vapor synthesis (MVS). The composition and structure of iron-containing fluoropolymer is studied by transmission electron microscopy and X-ray photoelectron and Mossbauer spectroscopy. Fe nanoparticles with an average size of 9 nm, consisting of ∼30% FeO and ∼70% Fe3+, are registered in the sample. Fe0 nanoparticles are stabilized in fluoropolymer pores and are coated with nanoparticles of nonstoichiometric iron oxides that have superparamagnetic properties.