This work describes a systematic study of gelatin-sepiolite structural bionanocomposites to show how the renaturation level of the biopolymer is highly dependent on the type of mineral particle used. The aim of the work is to prove that chemical interactions between both components (hydrogen and covalent bonding) determine the organization level of the biopolymer which in turn results in drastic differences in the elastic properties of the prepared bionanocomposites. To assess this, several systematic modifications were introduced into the silicate structure and surface, generating four derivatives. Two derivatives prepared by thermal treatments, monohydrated sepiolite and protoenstatite, and two chemically modified sepiolites, amino and epoxy terminated, were prepared and used as the inorganic (or hybrid) phase in the bionanocomposites. The thermal and chemical modifications performed on the sepiolite surface induced a dramatic decrease in the renaturation level as determined by DSC and FTIR techniques. On the other hand, untreated sepiolite induced a higher renaturation level in the polypeptide, probably due to the alignment of the collagen-like triple helix along sepiolite external surface channels. The measured mechanical properties of the studied compositions confirm that the renaturation level of gelatin is a key factor in understanding the elastic properties of bionanocomposites. These results suggest that mineral particles introduced in the polypeptide matrix provide an effective control over the matrix crystallinity giving rise to tunable mechanical properties of the final bionanocomposite. © the Owner Societies 2011.