Carbon nanotube (CNT)-filled epoxidized natural rubber (ENR) composites were prepared by mixing in an internal mixer and thereafter on a two-roll mill. Silane coupling agent, namely 3-aminopropyltriethoxy silane (APTES), was directly incorporated in the ENR-CNT composites during mixing of rubber and CNTs in the mixer, to perform in situ functionalization. It was found that pre-crosslinking of ENR and APTES occurred especially at high APTES concentrations, such as 0.06 mL/(g of CNTs) and caused strong CNT agglomeration in the ENR matrix. However, the pre-crosslinking could be reduced or avoided by decreasing the APTES concentration. In the concentration range 0.01-0.015 mL/(g of CNTs) of APTES, the APTES molecules were grafted on the CNT surfaces and generated new chemical linkages with the ENR. This improved the CNT dispersion in the ENR matrix and enhanced the composite properties. A very low approximately 0.5 phr of CNT threshold concentration for electric percolation was achieved in this type of composites. Also, threedimensional connected CNT networks were found to form in the ENR matrix at very low APTES levels. Thus, the electrical conductivity achieved in these composites reached the level required of conductive materials.