In this paper, firstly, the morphology and toughness of a range of bulk epoxy polymers, which incorporate a second phase of well-dispersed silica nanoparticles and/or rubber microparticles, have been determined. Secondly, the macro-properties of natural-fibre reinforced-plastic (NFRP) composites based upon these epoxy polymers have been ascertained, using (i) unidirectional flax fibres or (ii) regenerated-cellulose fibres in the architecture of a plain-woven fabric. Thirdly, the toughening mechanisms which are induced in these materials by the presence of the silica nanoparticles, the rubber microparticles and the natural fibres have been identified. Finally, the values of the toughness of the bulk epoxy polymers and corresponding NFRPs have been quantitatively modelled. The increased toughness recorded for the bulk epoxy polymer due to the presence of the silica nanoparticles and/or rubber microparticles was indeed typically transferred to the NFRP composites when using such epoxies as the matrices for the fibres. Thus, the important role that may be played by modifications to the epoxy matrices in order to increase the toughness of the composites was very clearly demonstrated by these results. However, notwithstanding, the toughening mechanisms induced by the fibres were essentially responsible for the very high toughnesses of the NFRP composites, compared with the bulk epoxy polymers. The modelling studies successfully predicted the values of toughness of the bulk epoxy polymers and of the NFRP composites. These studies also quantified the extent to which each toughening mechanism, induced by the second-phase nano- and microparticles and the natural fibres, contributed to the overall values of toughness of the materials.