This study investigates the augmentation of electrical and mechanical characteristics of natural rubber (NR) film with different forms by integrating carbon nanotubes (CNTs). NR with different forms (i.e., natural rubber grafted with polystyrene (NR–g–PS) and polybutyl methacrylate (NR–g–PBMA)) were successfully synthesized. The success of these grafting was confirmed through Proton Nuclear Magnetic Resonance (1H–NMR) and Attenuated Total Reflectance–Fourier Transform Infrared (ATR–FTIR) analyses, which showed that the grafting efficiency exceeded 90%. The properties of ungrafted NR and grafted NRs with CNTs were compared and analyzed. It was found that the NR/CNTs composites with grafting displayed significantly improved electrical properties and mechanical strength when compared to the NR/CNTs composites without grafting. It was found that the NR–g–PBMA exhibited an 860% increase in electrical conductivity at 100 kHz compared to ungrafted NR. This might be attributed to the synergistic of the high specific surface of CNTs and the high polarization of functional groups, which gave a higher value for the CNTs filled grafted NR than the ungrafted NR. Moreover, the mechanical properties of NR–g–PS composites showed a 114% increase in 100% modulus, 127% in tensile strength, and 37% in hardness, while the NR–g–PBMA composites exhibited a 159% increase in 100% modulus, 95% in tensile strength, and 34% in hardness compared to ungrafted NR. This enhancement can be attributed to the formation of chemical linkages between the grafted NR matrix and CNTs through functional groups from both. Consequently, it can be concluded that introducing functional groups on grafted NR assists in establishing a crosslinking network, enhancing both the mechanical and electrical properties. Additionally, this research emphasizes the benefits of producing flexible conductive materials with high modulus and enhanced electrical properties. Keywords: Natural rubber latex, Graft copolymerization, Glutaraldehyde, Natural rubber composites, Electrical properties