AbstractIn this novel work, we fabricated the multiwalled carbon nanotubes (MWCNTs)/polypyrrole (PPy) nanocomposite by employing the novel ultrasonic dual mixing (UDM) method. Subsequently, the atomistics and structural characterizations of the fabricated MWCNT/PPy nanocomposite (PM) were performed using SEM, Raman, and XRD. Furthermore, we experimentally evaluated the mechanical properties of the fabricated PM by reinforcing the PPy matrix with MWCNTs at different wt.%. The experimental study of PM shows that the mechanical properties depend upon the amount and dispersion quality of MWCNTs in the PPy matrix. In order to validate the experimental outcomes, the conservative fully coupled finite element (FE) models were developed using the ANSYS Workbench and novel FEAST software. The electromagnetic interference (EMI) shielding effectiveness (SE) of developed PM was also calculated at different thicknesses of PM by taking the effect of SE due to absorption (SEA) and SE reflection (SER) in the microwave frequency range of the C‐band (5.37–8.2 GHz) into consideration. The total SE (SET), the cumulative sum of SEA and SER, is the strong function of the thickness of the PM. Additionally, our study's outcomes reveal that as the thickness of the PM increased, the SET also increased by dominating the SEA rather than the SER. The SET value of 75 dB was observed for a sample with a thickness of 3 mm, indicating a high level of shielding. Thus, material becomes a highly attractive option for achieving high‐performance EMI SE in the C‐band for satellite communications, Wi‐Fi devices, weather radar systems, surveillance, and cordless telephones. A complex permittivity and permeability were also studied using the Nicolson–Ross–Weir (NRW) method to understand the mechanism behind the EMI SE.Highlights Nanocomposite fabricated using the novel ultrasonic dual mixing method. FE models were developed to validate experimental results. The EC and EMI SE are improved with the increase in the sample thickness. Absorption, rather than reflection, dominated the shielding mechanism. SE was observed dB with good mechanical properties.