Iron–alumina composites consisting of different loadings of iron particles dispersed in an alumina matrix were prepared via a facile impregnation–calcination process. The frequency dispersions of conductivity and permittivity were investigated in detail. An ultra low percolation threshold of 2.3 vol%, which is much lower than that of dense metal–ceramic composites, was obtained. Meanwhile, a significant enhancement of permittivity ε′ (from ∼7.5 to ∼800) was achieved when the iron content increases from 0 to 4.2 vol% at 10 MHz. The ultra low percolation threshold can be explained by the fact that the porous microstructure of the composites will facilitate the formation of a layer of two dimensional conductive networks on the pore wall of porous alumina. And the significant enhancement of permittivity should be attributed to the interfacial polarization phenomenon that takes place at the iron–alumina interfaces. This paper demonstrates that the loading of a conductive component into a porous matrix is an effective way to fabricate composites with simultaneously high permittivity and ultra-low percolation threshold. Hopefully, various porous metal–ceramic composites with tailored dielectric properties could be fabricated using the impregnation–calcination process.