Moso bamboo (Phyllostachys edulis), an apt example of an anisotropic, functionally graded composite material, is the most important commercial bamboo species of China. This species has excellent mechanical properties due to its unique vascular bundle structure. This article examines the variation in mechanical properties of single vascular bundles with respect to their location within a bamboo culm. The mechanical exfoliation method was used to prepare the single vascular bundle. This study found that moso bamboo has superior stiffness and strength. Additionally, the variation in properties was large in the radial direction but minimal in longitudinal direction. The large variation in mechanical properties of vascular bundles can be ascribed to the synergistic effect of the fibrous sheath and parenchyma rather than to changes in fibrous sheath properties. This study provides a basis for the structure application for moso bamboo.