In this study, multiwalled carbon nanotubes (MWCNTs) were incorporated into vulcanized natural rubber (VNR) matrixes to create nanocomposites with improved mechanical, thermal, and electrical properties. The interfacial interaction of the MWCNTs with the VNR matrix was quantitatively evaluated based on the crosslink density value calculated using the Flory–Rehner methodology. Various rheometric parameters were influenced by the addition of the MWCNTs, including minimum torque (M_L), maximum torque (M_H), and scorch time (t_S1). The MWCNTs significantly enhanced the vulcanization of the composites based on the VNR matrix. This study highlights the impact of MWCNTs on crosslink density, improving mechanical properties and reducing swelling in the VNR matrix. We discovered that the MWCNTs and the VNR matrix interact strongly, which improved the mechanical properties of the matrix. The MWCNTs improved the hardness, tensile strength, and abrasion resistance of the VNR/MWCNT nanocomposites. Based on dynamic mechanical analysis, MWCNT incorporation improved stiffness as indicated by a change in storage modulus and glass transition temperatures. The addition of MWCNTs to the VNR/MWCNT nanocomposites significantly improved their electrical properties, reaching a percolation threshold where conductive pathways were formed, enhancing their overall conductivity. Overall, this study demonstrates the versatility and functionality of VNR/MWCNT nanocomposites for a variety of applications, including sensors, electromagnetic shielding, and antistatic blankets.