Thin multilayer structures consisting of a nanocomposite CrZr x alloy on SiO 2 are grown by magnetron sputtering onto hard-coated polymeric substrates at 350 K. The grain structure and electrical, optical, and mechanical properties of the nanocomposite alloy were investigated using atomic force microscopy, dc conductivity, spectrophotometry, and nano-scratch testing. Despite the sputtered films being grown in the same deposition run, the grain structure and properties of the thin films were observed to change depending on the siloxane-based hard-coat employed. These studies indicate that in addition to the substrate's roughness, the hardness of the siloxane-based hard-coat correlates well with the changing properties of the sputtered thin films. To rationalize the influence of the substrate hardness, a hypothesis is proposed where the substrate hardness dissipates a portion of the sputtered material's energy upon impact, leading to changes in its residual energy, thus influencing the material's ability to laterally diffuse on the substrate.