Abstract: The three-dimensional hierarchical structure of collagen fiber (CF) has the natural advantage of resilient creep-resistant modification of polyvinyl chloride (PVC), but the hydrophilic CF is difficult to be compatible with the hydrophobic PVC effectively, which limits the modification efficacy of PVC by CF. Modified CF (M-CF) was prepared with amino-silane coupling agent (APTES). The structural transformation pattern of M-CF, and the structure, creep behavior, and fracture behavior of M-CF/PVC were investigated by field emission scanning electron microscopy, Fourier transform infrared spectroscopy, and dynamic mechanical analysis. The results show that APTES improves the hydrophobicity of CF and formed ionic and covalent bonds with PVC chains, thereby greatly improving the compatibility between CF and PVC. In addition, APTES modification fully opens the three-dimensional hierarchical structure of M-CF, which allows PVC to better penetrate into theM-CF phase region and form more blocking sites between PVC and M-CF. As a result, the movement of PVC chains is obviously inhibited, the deformation activation energy of M-CF/PVC is increased by 30.7% compared with that of pure PVC, the creep lifetime of M-CF/PVC is extended to 80.5 times than that of pure PVC and 2.3 times that of CF/PVC, and the reversible deformation (11.50%) of M-CF/PVC is increased to more than 1.4 times than that of the conventional modified PVC. In summary, the improved compatibility between CF and PVC endows M-CF/PVC with ideal resilient creep-resistance.