Reversibly crosslinked blends of isotactic polypropylene and low density polyethylene (iPP/LDPE) were prepared in the presence of crosslinking agents using reactive extrusion. The structure and properties of the modified blends were investigated by means of wide-angle X-ray scattering (WAXS), differential scanning calorimetry (DSC), and macro- and micro-mechanical measurements. The crystallinity of the modified samples (LDPE, iPP, and their blends) does not seem to be so much affected by the crosslinking process. Results show that the microhardness of the iPP/LDPE blends notably increases with the iPP content. The micromechanical properties of the modified blends only improve slightly as a consequence of the crosslinking process. In the iPP samples, and also in the iPP/LDPE blends, this process gives rise to the appearance of new, crystalline ethylenic chains, as evidenced by the calorimetric measurements. Furthermore, the impact strength of the modified materials is improved as compared with that of the original ones, while some of the crosslinked blends show a ductile fracture behavior. (C) 2008 Wiley Periodicals, Inc.