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The mechanical properties of fiber composites are greatly affected by the interfacial interactions between the fibers and matrix, and hence the study of interfacial properties becomes critical. This study demonstrates a simple and effective interfacial modification process using polydopamine (PDA) coating with ZnO nanorods to construct a multi‐scale bionic structure on the polyacrylonitrile (PAN) fiber, which is conducive to increasing the bonding area and enhancing the load transfer, thus boosting the mechanical properties of the modified fiber‐incorporated asphalt binder. The cone penetration test and thermogravimetric analysis show that the octopus‐inspired multiscale PAN fiber (OIM‐PAN) composite styrene butadiene styrene modified binder (SBS/MB) has better shear strength and thermal stability. Dynamic shear rheometer test shows that the deformation resistance and viscoelastic properties of the fiber composite SBS/MB are enhanced compared with SBS/MB, and the OIM‐PAN composite SBS/MB (OIM‐PAN@SBS/MB) exhibits the best deformation resistance and viscoelastic properties. Thus, it can be concluded that this interfacial modification process can significantly improve the mechanical properties of fiber–asphalt composites by introducing a third phase between the fiber and asphalt interface to achieve functionally graded material properties and enhance the load transfer between the interfaces for large‐scale applications in road engineering and construction sites.

Herein, tannic acid‐terephthalyl chloride (TA‐TPC) was prepared and was applied for the preparation of TA‐TPC‐Rubber to composite styrene butadiene styrene (SBS)‐modified asphalt (SBSMA). Fourier transform infrared spectroscopy and scanning electron microscopy indicated that TA‐TPC successfully attached to the surface of rubber powder (RP), which improved the bonding between RP and SBSMA. Fluorescence microscopy analysis showed that TA‐TPC‐Rubber formed a complete crosslinking network structure in SBSMA, while thermogravimetry analysis proved the higher thermal stability of TA‐TPC‐Rubber/SBSMA. Dynamic shear rheometer and multi‐stress creep recovery tests confirmed that compared with SBSMA, the storage modulus (G') and loss modulus (G") of 12% TA‐TPC‐Rubber/SBSMA at 46°C were increased by 37.14% and 34.36%, respectively, the recovery rate was increased by 35.49% (0.1 kPa) and 31.91% (3.2 kPa) while the average creep compliance was decreased by 68.67% (0.1 kPa) and 59.87% (3.2 kPa). The phase segregation test proved that the compatibility between RP and SBSMA was improved by the modification of TA‐TPC, and the difference between the upper and lower softening points were reduced by 53.85%. The findings of this study can be of great significance for designing modified asphalt from cost‐effective raw materials through a convenient process for highways and construction applications.

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