The relationships of the dielectric properties and structure of polypropylene (PP)/ nylon (Ny) blends containing carbon black (CB) were studied. Dielectric anisotropy was found in blends exhibiting an oriented fibrillar Ny network covered by CB particles. In the Ny fibril direction the composites are conductive, while in the perpendicular direction they are insulating, as indicated by the different frequency dependence of the AC conductivity in the two orthogonal directions. However, once CB is located within both the Ny and the PP the dielectric behavior is isotropic. This was further confirmed by Cole-Cole plots, which, for the first time, were found to fit numerical predictions of the "resistor-capacitor" (RC) model. The CB network formed upon the surface of the Ny fibrils is denser and/or better structured than that formed within the Ny phase. Thus, the former can be envisioned as a 2D system, as suggested by the values of the scaling exponents of the AC conductivity and permittivity with frequency, which have a lower activation energy for charge transport. The dielectric measurements were found helpful in elucidating the CB network structure.