In order to advance towards more sustainable electronics generation, natural polymers with tailored dielectric response are essential. In this search, the combination of bio-based materials with active fillers in composite form, suppose one of the most viable alternatives. To achieve it, this work has explored the ability to control dielectric response of Silk Fibroin, a protein polymer by its combination with ceramic barium titanate (BaTiO3) nanoparticles. Both the effect of filler concentration (0, 5, 10, 20 and 40 wt%) and size (100 and 200 nm) has been studied in composites processed by easily scalable techniques. Samples with a homogeneous distribution of nanoparticles have been obtained. Dielectric relaxation processes assessed by bro...