AbstractNatural fibres are partly replacing currently used synthetic fibres as reinforcement for polymer composites. Jute fibre bundles were high-cellulose-content modified by alkali treatment, while the bagasse fibre bundles were modified by creating quinones in the lignin portions of fibre surfaces and reacting them with furfuryl alcohol (FA) to increase their adhesiveness. The effects of different fibre bundle loading and modification of bagasse fibre surfaces in hybrid fibre reinforced epoxy composites have been studied. The role of fibre/matrix interactions in chemically modified hybrid composites were investigated using Differential Scanning Calorimeter, Differential Thermo Gravimetry, and a Universal Tensile Machine and compared with those of unmodified bagasse fibre bundles incorporated with modified jute fibre bundles reinforced hybrid composites. Fibre surface modification reduced the hydrophilicity of fibre bundles, and significantly increased mechanical properties of hybrid composites were observed in conjunction with SEM images. The SEM analysis of the fibre and the composite fractured surfaces have confirmed the FA grafting and shown a better compatibility at the interface between chemically modified fibre bundles and epoxy resin. This paper incorporates interesting results of thermomechanical properties and evaluation of fibre/matrix interactions.