In situ microfibrillar composites (PP/mPA66) of modified polyamide66 (mPA66) with polypropylene (PP) were prepared by using a post-compatibilization technique. The mPA66 was firstly obtained by reactive extrusion of PA66 resin with a specially designed compatibilizer, which was then blended with PP through extrusion combined with a hot stretching and subsequently quenching process. The PP/mPA66 in situ microfibrillar composites were comparatively studied with simply blended samples of PP/PA66 that were prepared by blending PA66 and PP together with (or without) the same compatibilizer through extrusion. PA66-g-PP (and/or elastomers) graft copolymer formation in mPA66 was identified by dissolution test and infrared spectroscopy measurement, the compatibilizer is unevenly dispersed with large domains in PA66 as observed by scanning electron microscope (SEM). In PP/mPA66 composites, the in situ generated PA66 microfibrils have a rather nonuniform diameter distribution and a very rough surface. SEM observations for the fractured surface illustrated that PP/mPA66 composites have structural characteristics of stronger adhesion and moderate flexibility of the interface. Enhanced compatibilization between the PA66 microfibrils with the PP matrix resulted in improved mechanical properties of the PP/mPA66 composites. With optimized composition, the PP/mPA66 composite has notched Izod impact strength, flexural modulus, and tensile yield stress of 1.49, 1.16, and 0.99 times as those of the neat PP, respectively. Such enhanced mechanical properties balance and improved interface adhesion were not found in the simply blended samples of PP/PA66 with or without the specially designed compatibilizer. (c) 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013