Compatibilized blends of polyamide-6 (PA6) and thermotropic liquid crystalline polymer (LCP) modified with various high-impact polypropylene (HIPP) contents were injection-molded. These blends were compatibilized with maleic anhydride-grafted polypropylene (MAP). The effects of impact modification on the morphology, impact, static, and dynamic mechanical properties were investigated. The results showed that the HIPP addition leads to an improvement of the Izod impact strength of the blends significantly while it reduced the tensile strength and stiffness properties. An attempt was made to correlate the structure of the PA6(MAP)/HIPP/LCP blends from the scanning electron microscopic observations with the measured mechanical properties. This work provides a way to produce a tough in situ composite.