Composite metal–polymer thin films were formed by implantation of 40 KeV Fe + and Co + ions into viscous and solid silicone substrates in the dose range of (0.3–1.5)×10 17 ions/cm 2. Morphology and magnetic properties of the synthesized films were investigated. TEM investigations showed that the microstructure of metal granular layers synthesized in silicone polymers strongly depends on an initial relaxation state of the target. Magnetic resonance studies revealed essential differences in the magnetic properties of thin metal films synthesized at different initial states of silicone substrate and with respect to the type of implanted ions (Fe or Co). A shift and broadening of FMR signal with the samples cooling are observed both for perpendicular and parallel orientation of the films with respect to the magnetic field. These effects are associated with the increase of the inter-particle interactions and superparamagnetism blocking in the particles. It was found that the viscous initial state of the polymer is a favourable factor for the high anisotropy of FMR response in Fe-implanted samples in contrast to the Co-based ones. The reasons for this have been discussed with respect to the morphology of Fe and Co synthesized films.