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We present an experimental and theoretical exploration of well‐dispersed, distinctively stable, fumed SiO2 crosslinked polyethylene (XLPE) nanocomposites. The mechanical properties of fumed SiO2 /XLPE nanocomposites were assessed with different concentrations of fumed SiO2, which had noticed that network morphology was immensely influential for the performance of mechanical properties. A reasonable exploration of micromechanical models of composites indicated that the theories of Nicolais–Narkis, and Pukanszky provided an excellent fit to yield strength data of the composites considering the effect of the interphase between XLPE and SiO2. Furthermore, it highlights that the experimental data can be superimposed with the static micromechanical models of Nicolais–Narkis, and Pukanszky. Owing to the proper dispersion of the SiO2 nanospheres in the XLPE matrix, the filler‐polymer interactions are found to be enhanced. Moreover, it resulted in the excellent insulation properties of the nanocomposites, which makes it a better candidate for electrical cable insulating materials. The combined results of structural characterizations by Fourier Transform Infrared Spectroscopy (FTIR), X‐Ray Diffraction (XRD), Differential Scanning Calorimeter (DSC), Dynamic Mechanical Analysis (DMA), Atomic Force, and Transmission Electron Microscopy (AFM, TEM) confirmed the role of fumed SiO2 as a reinforcing mediator in the current system.

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