The structure and mechanical properties of bio-nanocomposite films made from poly(ethylene oxide) (PEO) that is physically cross-linked with silicate nanoparticles, Laponite, are investigated. Direction-dependent mechanical properties of the films are presented, and the effect of shear orientation during sample preparation oon tensile strength and elongation is assessed. Repeated mechanical deformation results in highly extensible materials with preferred orientation and structuring at the nano- and micrometer scales. Additionally, in vitro biocompatibility data are reported, and NIH 3T3 fibroblasts are observed to readily adhere and proliferate on silicate cross-linked PEO while maintaining high cell viability.