Carboxyl-terminated poly(acrylonitrile-co-butadiene) (CTBN)-grafted epoxidized linseed oil (ELO) (CTBN-g-ELO) was synthesized and used as an effective toughener to simultaneously enhance the mechanical properties and fracture toughness of epoxy resin (EP). The ELO was fabricated from linseed oil via epoxidation processing. The characteristics of the ELO and CTBN-g-ELO, such as the average molecular weight and chemical structure, were determined using gel permeation chromatography, proton nuclear magnetic resonance, and Fourier transform infrared spectroscopy. The effects of the CTBN-g-ELO loading on the characteristics of the EP were investigated in detail. The test results indicated that by adding 15 phr CTBN-g-ELO, the tensile strength, impact strength, and critical stress intensity factor (K IC ) were significantly increased, by approximately 23.62, 91.8, and 33.8%, respectively, compared with pristine EP. The glass-transition temperature (T g ) and storage modulus, which were examined via dynamic mechanical thermal analysis and differential scanning calorimetry, respectively, exhibited decreasing trends. Scanning electron microscopy revealed that the CTBN-g-ELO existed as spherical particles in the EP, helping to stop the crack growth and change the crack growth directions.