Addition of β-form nucleating agent (β-NA) to isotactic polypropylene (iPP) can greatly induce the variation of the crystallization of matrix. Here, we introduce high pressure to the crystallization process of β-NA nucleated iPP. It is observed that there is a competition between the effect of high pressure and the nucleation effect of β-NA on crystallization of iPP. With the increasing of high pressure, both the contents of β-iPP and α-iPP decrease while the content of γ-iPP increases. A novel crystalline morphology of γ-iPP with the fragmentations of γ-spherulites regularly organized in a local region is observed. Namely, γ-spherulites grow on the lateral of β-NA needlelike structure. The dual nucleation effects of the special needlelike structure of β-NA towards β/α-iPP and the effect of high pressure which prevents the growth of β-iPP but promotes the growth of γ-iPP are the main mechanisms for the novel crystalline morphology of γ-iPP. Specifically, the mixed polymorphic β/γ-iPP can be achieved under a certain pressure. This possibly enlarges the application of iPP material.