Nanostructured poly(vinylidene fluoride) (PVDF)/acrylic rubber (ACM) blends have been prepared by simply melt blending of PVDF and several percent of ACM. The morphology and properties of the prepared nanoblends have been investigated by means of transmission electron microscopy (TEM), dynamic mechanical analysis (DMA), differential scanning calorimetry (DSC), and polarized optical microscopy (POM). It was found that ACM has been precisely dispersed in PVDF matrix with most of the particle size of less than 100 nm. The prepared nanoblends show a unique balance between the toughness and the stiffness. The impact strength and elongation at break of the nanoblends by adding small amount of ACM increase greatly, while there is only a little decreasing in the modulus, by comparing with neat PVDF. The investigation results indicate that the nanodispersed ACM domains not only take the role of the toughening agent for PVDF but also markedly increase the crystallization speed and reduce the spherulite size of PVDF, which also contributes greatly to the enhancement of the impact strength and elongation at break.