Metallocene-made isotactic polypropylene (m-iPP) exhibits better performance than the conventional Ziegler-Natta isotactic polypropylene in the areas of spinning and injection. In addition, the molecular chain structure features of m-iPP promote formation of γ-crystals. And manipulation of the crystallization kinetics and morphology of γ-crystal under the flow field are the foremost ways to tune and improve the performance of m-iPP. However, the related research is still in the primary stage. Combined effects of shear flow and non-isothermal process on the crystallization behavior of m-iPP simulating industrial processing were investigated by in-situ synchrotron wide-angle X-ray diffraction (WAXD) and small-angle X-ray scattering (SAXS) techniques. In terms of sheared sample, SAXS patterns clearly showed an evolution of ordered structure at the early stage of crystallization, while the corresponding WAXD patterns exhibit only α-crystals. SAXS at later stage of crystallization showed that part of ordering structure relaxed back to random coil, while emergence of γ-crystals was observed in WAXD patterns. Combined SAXS and WAXD result indicated that shear-induced ordered structures and the resulting relaxation behavior determined, under specific circumstances, α-crystals emerge and subsequent γ-crystals obtain the ability to appear. Unexpectedly, the final γ-crystal content was higher in the sheared samples than the static ones at a given cooling rate, which is attributed to the fact that the shear-induced the crystallization takes place at the range of γ-crystal favorable temperature, i.e., around 135 oC. Moreover, γ-crystal could serve as a good detector, which verified that shear could not only affect the crystallization nucleation and resulting relaxation in the early crystallization stage, but also should be the thermodynamics of subsequent full-scale crystallization. A mechanistic pathway for the crystallization development of sheared sample is proposed. Those results are of valuable guidance to tailor the interior structure of m-iPP during practical processing and hence to acquire desired properties of products.