The influence of boehmite crystallite sizes, varied between 10 and 60 nm, was studied with respect to the morphology development, crystallization behavior and mechanical properties of the boehmite‐based iPP nanocomposites. The nanometer‐scaled boehmites were formed during twin‐screw melt extrusion of iPP at 200 °C. Even in the absence of polymer compatibilizers, the boehmites, obtained from Sasol's process, enabled very effective deagglomeration and in‐situ dispersion of nanoboehmites. With increase in boehmite crystallite size it was possible to improve simultaneously stiffness and impact strength of iPP. As evidenced by means of DSC, POM and WAXS measurements, the deagglomerated nanoboehmites nucleated crystallization of poly(propylene)'s α‐modification.