An isotactic polypropylene (iPP) nanocomposite with low percolation threshold, ultrahigh dielectric permittivity and toughness by controlling the dispersion of multi-walled carbon nanotubes (MWCNTs) through ethylene-α-octene block copolymer (OBC), is reported. A special ‘sosatie’ structure, i.e. finely dispersed long MWCNTs inserted in OBC phase uniformly distributed in the continuous iPP matrix, was constructed through simple melt compounding process. The percolation threshold of the prepared iPP/OBC/MWCNT nanocomposites was ca. 0.5 vol.%, lower than that of iPP/MWCNT nanocomposites. The iPP/OBC/MWCNT nanocomposites exhibited an ultrahigh dielectric permittivity (ca. 9000) at 100 Hz and a very low dielectric loss (ca. 1.5). MWCNTs also improved the compatibility between iPP and OBC components, leading to a high impact strength of iPP/OBC/MWCNT nanocomposites (about 13 times higher than pure iPP when the content of MWCNT was 1.49 vol.%). Thus, the approach reported in this work can provide a new and convenient route to prepare high-performance polymer nanocomposite dielectric materials with low percolation thresholds and balanced mechanical properties.