Growing environmental concerns and stringent waste-flow regulations make the development of sustainable composites a current industrial necessity. Natural fibre reinforcements are derived from renewable resources and are both cheap and biodegradable. When they are produced using eco-friendly, low hazard processes, then they can be considered as a sustainable source of fibrous reinforcement. Furthermore, their specific mechanical properties are comparable to commonly used, non-environmentally friendly glass-fibres. In this study, four types of abundant natural fibres (jute, kenaf, curaua, and flax) are investigated as naturally-derived constituents for high performance composites. Physical, thermal, and mechanical properties of the natural fibres are examined to evaluate their suitability as discontinuous reinforcements whilst also generating a database for material selection. Single fibre tensile and microbond tests were performed to obtain stiffness, strength, elongation, and interfacial shear strength of the fibres with an epoxy resin. Moreover, the critical fibre lengths of the natural fibres, which are important for defining the mechanical performances of discontinuous and short fibre composites, were calculated for the purpose of possible processing of highly aligned discontinuous fibres. This study is informative regarding the selection of the type and length of natural fibres for the subsequent production of discontinuous fibre composites.