Co-decomposition of gaseous mixtures of silacyclopent-3-ene and Fe(CO) 5 by irradiation at (9 + 10) and (9 + 10 + 5) mm from two CO 2 lasers is reported. In a one-step process, this produced nanosized (a-Fe)-based particles that consist of both superparamagnetic and ferromagnetic phases. They were enveloped within a thin graphitic shell and embedded in an organosilicon polymer matrix. Properties of the nanocomposites, examined by infrared and Raman spectroscopies, high resolution transmission electron microscopy and magnetization studies, are shown to differ for the 2l and 3l irradiations. The latter consist of smaller Fe-based nanoparticles, display less graphitic carbon, possess more abundant Si/C/H phases and have their cores richer in Fe and superparamagnetic phase.