Sponge-like nanocomposites based on bacterial cellulose and silk fibroin (BC/SF:25%, BC/SF:50% and BC/SF:75%) were developed in this work. SEM evaluation results exhibit a very well interconnected porous network structure and large aspect of all nanocomposites produced. It could be demonstrated that the presence of fibroin influenced BC/SF scaffolds surface covering and this aspect was affected by fibroin concentration. The best outcome obtained is related to 50% fibroin content, where the equal ratio let to a very good symbiotic effect, preserving the specific properties of BC and SF. Bradford assay demonstrated that BC/SF:50% nanocomposite is stable. The results for cell adhesion assay showed that the presence of fibroin induced a significant increase on cell adhesion (BC/SF:50%) compared to pure BC membranes, due to the biologic nature of SF coating. Cytotoxicity assays demonstrated that the material is non-cytotoxic and Trypan Blue associated to the SEM images revealed that BC/SF:50% scaffolds present higher rates of cellular viability than pure BC. Further, it was found that the prepared BC/SF:50% scaffold led to an improved biocompatibility