An improved method to evaluate Young's modulus of bacterial cellulose (BC) nanofibrils is presented. This estimation takes into account polarisation configurations, nanofibril orientation and tensile deformation axis direction. A range of 79 - 88 GPa has been obtained showing their great potential to be used as reinforcement in composite materials.BC bio-composites, constituted of a BC layer embedded in-between two matrix layers, have been prepared by compression moulding. The stress-transfer from the matrix to the reinforcement has been quantified using Raman spectroscopy. This has been carried out by following the shift of the Raman band initially located at a wavenumber position of ~1095 cm-1. Polylactide (PLA) was chosen as matrix material due to its biodegradability and bio-sourced origin. Transparent polylactide films were obtained in specific processing conditions to suppress crystallisation. This allowed the laser to penetrate the matrix and interact with the upper layer of BC networks. Several factors that could affect the interface in these composites have been studied.The influence of the culturing time of BC networks on the composite interfaces has been investigated. Higher Raman band shift rates with respect to strain and stress have been measured for composites manufactured using BC networks having a low culturing time. This led to enhanced coupling between PLA and the upper layer of BC networks. Scanning electron microscopy imaging of the tensile fracture surface of these composites revealed that delamination between the BC layers was occurring rather than failure at the BC/PLA interface.Cross-linking of BC networks using glyoxal was performed to consolidate their layered structure. Raman spectroscopy was used to probe the stress-transfer of unmodified and cross-linked BC networks. These data revealed that cross-linked materials exhibit an enhanced stress-transfer both in the dry and wet states compared to unmodified BC networks.Cross-linked BC networks were used to design composites but no significant stress-transfer improvement was observed. As a result, maleated polylactide (MAPLA) was produced and used as a matrix material in order to consolidate the interface between PLA and both the upper and lower layer of cross-linked BC networks. Composites designed using cross-linked BC networks and MAPLA showed a significant stress-transfer improvement over composites designed using unmodified BC networks and PLA. Also the determination of the bulk tensile mechanical properties of the composites revealed a significant increase of relative Young's modulus. This increase is thought to be due to reduced molecular mobility at both the cross-linked BC/MAPLA interface and between cross-linked BC layers. This is further supported by scanning electron imaging of the tensile fracture surfaces.