In this study, bamboo fiber bundle‐reinforced composites (BFCs) were prepared from Neosinocalamus affinis and phenol‐formaldehyde resins. The strength and modulus of BFC were more than double those of the raw bamboo. By using micro computed tomography, scanning electron microscopy and nanoindentation tests, the reinforcement mechanism of the bamboo‐based composites was investigated. And the details were summarized as follows. As the strongest parts of bamboo, the mechanical properties of the fiber cells were almost unchanged but their relative amounts increased due to the densification, thereby improving the carrying capacity. The ground tissues, the weakest parts of bamboo, had a substantial improvement in their mechanical properties. Due to elaborative fluffing process and high pressure forming, the intercellular space and cell cavity were filled with resins. The resins bonded the ingredients together so that the weak intercellular layers were enhanced. POLYM. COMPOS., 40:1463–1472, 2019. © 2018 Society of Plastics Engineers