It has been demonstrated by researchers that the β-form is beneficial to toughness and ductility. In addition, the transcrystallinity (TC), which shows highly oriented columnar morphology considerably different from the spherulitic crystal growth commonly encountered in PP, had been investigated for a long time because the formation of TC can improve the interfacial properties and various mechanical properties. Therefore, some works had been done on preparing β-transcrystallinity(β-TC). However, no matter what kinds of methods were applied to induce β-TC, the obtained β-TC was low content, discontinuous, and ranged randomly in the whole system. In order to obtain massive, continuous and highly ordered β-TC, the β-nucleated polypropylene (β-PP) and polypropylene (PP) with alternating layers were prepared by multilayered coextrusion technology. The transcrystallization which was induced by β-nucleating agents (β-NA) was observed at the interface. The β-TC structures were investigated by differential scanning calorimeter (DSC), Polarized optical microscopy (POM), scanning electron microscopy (SEM), wide-angle X-ray diffraction (WAXD) and microscopic fourier transform infrared spectroscopy (Micro-FTIR). The crystallization behavior and formation mechanism of β-TC were investigated in this paper. The results indicated that the relative content of β-TC increased with the increasing number of layers. Further, the microstructure of β-TC was also observed and a structural model was proposed to describe a new crystalline morphology induced by β-NA. In addition, the lamellae orientation was detected, and the results show that the orientation was increased with the increasing number of layers. In this study, we provided a simple and convenient way to manufacture a PP material with high content of β-TC, and expand the potential application of β-TC.