We present a novel bionanocatalyst fabricated by the adsorption-reduction of metal ions on a polyurethane/S-layer protein biotemplate. The bioinspired support was obtained by the adsorption of S-layer proteins (isolated from Lentilactobacillus kefiri) on polyurethane particles. Silver and platinum nanoparticles were well-loaded on the surface of the support after the combination with metallic salts and reduction with H2 at room temperature. Transmission electron microscopy analysis revealed the strawberry-like morphology of the bionanocatalysts with a particle size, dn, of 2.39 nm for platinum and 9.60 nm for silver. Both systems catalyzed the hydrogenation of p-nitrophenol to p-aminophenol with high efficiency in water at mild conditions in the presence of NaBH4. Three different amounts of bionanocatalyst were tested, and in all cases, conversions between 97 and 99% were observed. The catalysts displayed excellent recyclability over ten cycles, and no extensive damage in their nanostructure was noted after them. The bionanocatalysts were stable during their production, storage, and use, thanks to the fact that the biosupport provides an effective driving force in the formation and stabilization of the metallic nanoparticles. The successful bioinspired production strategy and the good catalytic ability of the systems are encouraging in the search for nontoxic, simple, clean, and eco-friendly procedures for the synthesis and exploitation of nanostructures.