It is a challenge to develop cost-effective strategy and design specific microstructures for fabricating polymer-based impact-resistance materials. Human shin bones require impact resistance and energy absorption mechanisms in the case of rapid movement. The shin bones are exciting biological materials that contain concentric circle structures called Haversian structures, which are made up of nanofibrils and collagen. The “soft and hard” structures are beneficial for dynamic impact resistance. Inspired by the excellent impact resistance of human shin bones, we prepared a sort of polyurethane elastomers (PUE) composites incorporated with rigid carbon nanofibers (CNFs) modified by elastic mussel adhesion proteins. CNFs and mussel adhesion proteins formed bone-like microstructures, where the rigid CNFs are served as the bone fibrils, and the flexible mussel adhesion proteins are regarded as collagen. The special structures, which are combined of hard and soft, have a positive dispersion and compatibility in PUE matrix, which can prevent cracks propagation by bridging effect or inducing the crack deflection. These PUE composites showed up to 112.26% higher impact absorbed energy and 198.43% greater dynamic impact strength when compared with the neat PUE. These findings have great implications for the design of composite parts for aerospace, army vehicles, and human protection.