Open‐cell, porous microcellular foams with nanofibrillated structures were prepared from high tacticity isotactic polypropylene (i‐PP) with a crystal nucleating and gelling agent. The 1,3:2,4 bis‐O‐(4‐methylbenzylidene)‐d‐sorbitol gelling agent (Gel‐all MD) was used as the crystal nucleating and gelling agent, which enhanced the crystallization and gelation of i‐PP with a three‐dimensional network of highly connected nanofibrils. The core‐back foam injection molding technique was employed to foam the i‐PP with nitrogen (N2) at a high expansion ratio, where the crystal nucleating agent induced bubble nucleation and bubble growth in the inter‐lamella region and opened the cell walls with a nanoscale‐fibrillated structure. The effects of the nucleating agent on the open cell content (OCC), density and crystallinity were thoroughly investigated. We prepared open‐cell micro/nanocellular foams with an average cell size of microscale voids of < 5 μm. Nanometer‐scale fibrillated structures were formed on the cell wall of the microscale void, the expansion ratio was five‐fold and the open cell content was over 90%. POLYM. ENG. SCI., 54:2075–2085, 2014. © 2013 Society of Plastics Engineers