Sustainable fibre reinforced polymer composites have drawn significant attention in many industrial sectors as a means for overcoming issues with end-of-life regulations and other environmental concerns. Plant based natural fibres are considered to be the most suitable reinforcement for sustainable composites since they are typically from renewable resources, are cheap, and are biodegradable. In this study, a number of plant based natural fibres-curaua, flax, and jute fibres-are used to reinforce epoxy, poly(lactic acid) (PLA), and polypropylene (PP) matrices to form aligned discontinuous natural fibre reinforced composites (ADNFRC). The novel HiPerDiF (high performance discontinuous fibre) method is used to produce high performance ADNFRC. The tensile mechanical, fracture, and physical (density, porosity, water absorption, and fibre volume fraction) properties of these composites are reported. In terms of stiffness, epoxy and PP ADNFRC exhibit similar properties, but epoxy ADNFRC shows increased strength compared to PP ADNFRC. It was found that PLA ADNFRC had the poorest mechanical performance of the composites tested, due principally to the limits of the polymer matrix. Moreover, curaua, flax (French origin), and jute fibres are found to be promising reinforcements owing to their mechanical performance in epoxy and PP ADNFRC. However, only flax fibre with desirable fibre length is considered to be the best reinforcement constituent for future sustainable ADNFRC studies in terms of mechanical performance and current availability on the market, particularly for the UK and EU.