Our purpose was to improve the thermal, mechanical and optimal properties of an epoxy bioresin using optimum hybrid natural pigments previously synthesised in our lab. Next, we searched for the best combinations of factors in the synthesis of natural hybrid nanopigments and then incorporated them into the bioresin. We combined three structural modifiers in the nanopigment synthesis, surfactant, coupling agent (silane) and a mordant salt (alum), selected to replicate mordant textile dyeing with natural dyes. We used Taguchi's design L8 to seek final performance optimisation. We selected three natural dyes, chlorophyll, beta-carotene and beetroot extract, and used two laminar nanoclay types, montmorillonite and hydrotalcite. The thermal, mechanical and colorimetric characterisation of the composite obtained by mixing natural hybrid nanopigments (bionanocomposite) was made. The natural dye interactions with both nanoclays improved the thermal stabilities, colour performance and UV-VIS light exposure stability of natural dyes and bioresins. The best bionanocomposite materials were found in an acidic pH [3, 4] environment and by modifying nanoclays with mordant and surfactant during the nanopigment synthesis process.