Iron/iron oxide-based nanocomposites were prepared by IR laser sensitized pyrolysis ofFe(CO)5and methyl methacrylate (MMA) mixtures. The morphology of nanopowder analyzed by TEM indicated that mainly core-shell structures were obtained. X-ray diffraction techniques evidence the cores as formed mainly by iron/iron oxide crystalline phases. A partially degraded (carbonized) polymeric matrix is suggested for the coverage of the metallic particles. The nanocomposite structure at the variation of the laser density and of the MMA flow was studied. The new materials prepared as thick films were tested for their potential for acting as gas sensors. The temporal variation of the electrical resistance in presence ofNO2, CO, andCO2, in dry and humid air was recorded. Preliminary results show that the samples obtained at higher laser power density exhibit rather high sensitivity towardsNO2detection andNO2selectivity relatively to CO andCO2. An optimum working temperature of200°Cwas found.