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The current work studied the physical modification effects of non-covalent surfactant on the carbon-particle-filled nanocomposite. The selected surfactant named Triton™ X-100 was able to introduce the steric repelling force between the epoxy matrix and carbon fillers with the help of beneficial functional groups, improving their dispersibility and while maintaining the intrinsic conductivity of carbon particles. Subsequent results further demonstrated that the physically modified carbon nanotubes, together with graphene nanoplates, constructed an effective particulate network within the epoxy matrix, which simultaneously provided mechanical reinforcement and conductive improvement to the hybrid nanocomposite system. For example, the hybrid nanocomposite showed maximum enhancements of ~75.1% and ~82.5% for the quasi-static mode-I critical-stress-intensity factor and dynamic compressive strength, respectively, as compared to the neat epoxy counterpart. Additionally, the fine dispersion of modified fillers as a double-edged sword adversely influenced the electrical conductivity of the hybrid nanocomposite because of the decreased contact probability among particles. Even so, by adjusting the modified filler ratio, the conductivity of the hybrid nanocomposite went up to the maximum level of ~10−1–100 S/cm, endowing itself with excellent electro-thermal behavior. [ABSTRACT FROM AUTHOR]