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Fabrication of the helical fibers with sheath/core structure comprising 3D interconnected porous polystyrene (PS) and ductile polyvinylidene fluoride is inspired by coiled plant tendril. The key innovation point applied in this study is to produce a helical porous system based on sheath/core structure that can come into being a huge storage space in the sorption process for crude oil. More importantly, the mechanical properties confirm to have a more excellent improvement than that of the initial PS fibers, which make it become a possible candidate for the large‐area sorption and reuse of crude oil from the ocean or industry. The bioinspired fabricating strategy opens a significant avenue between the coaxial electrospinning and crude oil contamination cleanup. It is also expected that the unique structure can make it a promising candidate for applications in energy conversion, tissue engineering, and intelligent devices.