Ziegler–Natta catalysts were supported on nanosized ferroelectric (Pb,Sr)TiO3 (PST) powders and then (Pb,Sr)TiO3/polyethylene (PST/PE) nanocomposites were prepared by in situ polymerization. PST/PE nanocomposites with different volume fractions of PST were obtained by changing the polymerization time. The dispersion and element distribution of PST powders in the PST/PE nanocomposite were investigated. The results indicated that PST homogeneously dispersed in the PE matrix and PST/PE nanocomposite was formed. Moreover, the dielectric constant of PST/PE appeared to have a strong concentration dependence.