Nanocrystalline α–Fe, Fe3C, and Fe7C3, particles with narrow size distributions were produced by CO2 laser pyrolysis of vapor mixtures of Fe(CO)5 and C2H4. Details of the synthesis procedure are discussed. Mossbauer spectroscopy and x-ray diffraction were used to identify the structural phases and the former was used also to study the magnetism of the nanoparticles. All the nanoparticles were observed to be ferromagnetic in this size range. If excess C2H4 appears in the reactant gas mixture, several monolayers of pyrolytic carbon were observed to form on the particle surface, as deduced from transmission electron microscopy and Raman scattering studies. Results of thermo-gravimetric analysis/mass spectroscopy studies of this carbon coating indicate it is gasified in hydrogen at temperatures T ∼ 250 °C.