The structure of jute fibre has been modified using caustic soda up to a limit in order to improve its performance. The SEM micrographs of untreated jute fibres show a smooth surface, while alkalised jute fibres show rough and void regions between individual fibre cells. The study showed that the tensile strength and Young’s modulus of jute fibre bundles depends on the physical characteristics of its internal structure such as the cellulose content, changes in the crystalline region content expressed in terms of crystallinity index, and micro-fibril angle. Results also showed tensile properties optimised at 0.24% NaOH (w/w). Overall, alkalised fibres exhibit brittle fracture. The study demonstrated the dependence of tensile properties on the changes in fibre structure following alkalisation.