The fabrication of miscible or nanostructured polymer blends or alloys raises much hope, but poses significant scientific and industrial challenges over the past several decades. Here, we propose a novel strategy using high-shear processing and demonstrate the high-shear effects on the nanodispersed structure formed in the poly(vinylidene fluoride) (PVDF)/polyamide 11 (PAll) blends, in which PA11 domains with a size of several tens of nanometers are dispersed in the PVDF phase. For the blend of PVDF/PA11 = 65/35, the TEM image shows that many nanometer-sized PAl1 particles are dispersed in the PVDF domain to form a special type of domain-in-domain morphology. In contrast, no PVDF nano-dispersion was observed in the PA11 phase. The effects of both the screw rotation speed and the mixing time on the blend structure were systematically studied. It shows that the extruder screw rotation speed and the mixing time are two critical factors to prepare the nanostructured blends. In addition, the investigations on the thermal behavior of the obtained blends indicate the improved miscibility between PVDF and PAl1 by the high shear processing.