Polyamide 6 (PA6)/poly(vinylidene fluoride) (PVDF) blend-based nanocomposites were successfully prepared using a twin screw extruder. Carbon nanotube (CNT) and organo-montmorillonite (30B) were used individually and simultaneously as reinforcing nanofillers for the immiscible PA6/PVDF blend. Scanning electron micrographs showed that adding 30B reduced the dispersed domain size of PVDF in the blend, and CNT played a vital role in the formation of a quasi-co-continuous PA6-PVDF morphology. Transmission electron microscopy observation revealed that both fillers were mainly located in the PA6 matrix phase. X-ray diffraction patterns showed that the presence of 30B facilitated the formation of γ-form PA6 crystals in the composites. Differential scanning calorimetry results indicated that the crystallization temperature of PA6 increased after adding CNT into the blend. The inclusion of 30B retarded PA6 nucleation (γ-form crystals growth) upon crystallization. The Young’s and flexural moduli of the blend increased after adding CNT and/or 30B. 30B exhibited higher enhancing efficiency compared with CNT. The composite with 2 phr 30B exhibited 21% higher Young’s modulus than the blend. Measurements of the rheological properties confirmed the development of a pseudo-network structure in the CNT-loaded composites. Double percolation morphology in the PA6/PVDF blend was achieved with the addition of CNT.