Herein, a series of multilayered materials consisting of alternating isotactic polypropylene (iPP) layers and cross-linked iPP (cPP) layers were fabricated via a multilayer coextrusion system. Ecstatically, a regular and symmetrical transcrystallinity (TC) structure with abundant beta-form crystals was constructed in iPP layers. Noticeably, the crystallization of cPP required a lower supercooling degree and the crystallization rate of cPP was faster than that of iPP. Accordingly, before iPP layers crystallized, numerous alpha-form crystals emerged at the interfaces within cPP layers, which could act as alpha-row nuclei. Under rapid cooling, closely packed beta-nuclei were induced near the interfaces via an alpha-to-beta transition, thereby facilitating the emergence of beta-form TC. Furthermore, by increasing layer numbers, the crystalline morphologies in iPP layers varied from a sandwich structure of TC/alpha-form spherulites/TC to a two symmetrical TC structure. Such a unique structure of a two symmetrical TC structure with abundant beta-phase may not only alleviate the stress concentration and cavitation caused by the existence of spherulites, but also increase the relative proportion of beta-form crystals in iPP layers, leading to the remarkable enhancement of strength and toughness. Therefore, this work provided an additive-free method to fabricate high-performance iPP products by constructing a continuous beta-TC structure.