During the “slit die extrusion-hot stretching” process, highly oriented polyamide 6 (PA6) dispersed phase was produced and retained in the polypropylene (PP) matrix directly. By adjusting the stretching forces, the PA6 spherical phase evolved into the ellipsoid, rod-like microfibril with a decreasing average diameter; then, the PA6 microfibrils broke. Moreover, the effects of the PA6 phases formed in the process of the microfibrillation on PP’s crystallization behaviors were studied systematically. As the stretching forces increased, the crystallization ability and orientation degree of PP crystals improved significantly. Differential scanning calorimetry and polarizing optical microscopy confirmed the formation of PP spherulite, fan-shaped lamellae and a transcrystalline layer under the induction of the PA6 phases with different morphology. In the PP/PA6 microfibrilar composites (MFCs), PP crystals showed smaller average size, more crystals and stronger interface adhesion due to more excellent heterogeneous nucleation ability of the PA6 microfibrils, which made contributions to the improvement of the melt elasticity responses and oxygen barrier properties of the PP/PA6 polymer blends.