Polypropylene/carbon nanostructure (PP/CNS) nanocomposite foams with a void fraction as high as 78% were successfully prepared by foam injection molding (FIM) with core-back operation. Rheological curves and differential scanning calorimetry results showed that the added CNS significantly improved the melt strength and accelerated the crystallization process of PP, respectively. A high mold temperature was applied to overcome the adverse effect of CNS, which had a high thermal conductivity and went against the preparation of high void fraction (VF) products. Thus, adding CNS could dramatically increase cell density by three orders of magnitude. With a CNS loading of 5 wt%, the PP/CNS nanocomposite foam with a cell size of about 60 μm, cell density over 10 7 cells/cm 3 , and a void fraction of 78% was obtained. More interestingly, the specific flexural modulus of the PP/CNS composite foam with 50% void-fraction was increased by 37% relative to the neat solid injection-molded PP. PP/CNS composite foams with adjustable cell structure and good mechanical properties show great potential for electromagnetic interference (EMI) shielding and sensors applications.