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Bamboo fiber is a prime green fiber due to its renewability, biodegradability, and high specific strength. Bamboo-fiber-reinforced epoxy (BFRE) composites have seen extensive use and shown great promise for natural biofiber-reinforced friction materials. Inspired by the decussated fiber alignment of bovine enamel, this study investigated how fiber orientation influences the tribological properties of BFRE composites. Specifically, the proportion of fibers oriented vertically to the surface was varied at seven levels: 0%, 25%, 33%, 50%, 67%, 75%, and 100%. The tribological performance was assessed through wear reciprocating testing and microscopic morphological characterization techniques. Results indicate that the bio-inspired fiber decussation can reduce the wear loss of the BFRE composites. Among all bio-inspired BFRE composites, BFRE composites with 67% vertical fibers achieve the best wear resistance. The vertical fibers in the BFRE composites can withstand pressure to provide a “compression–rebound” effect, while the parallel fibers can resist shear stress. The decussated structure inhibits crack initiation and propagation during wear and promotes transfer film formation, reducing wear loss. The findings expand understanding of the correlation between the bovine-tooth-like decussated structure and its tribological mechanisms, thereby offering essential guidance for the biomimetic design of high-performance BFRE composites for friction material application. Full article