AbstractCastor (Ricinus communis L.) stalk is a byproduct of the production of castor oil. As a natural material, castor stalk has great potential in the production of bio-composites as reinforcement materials. To provide more information about the castor stalk for using it better, the structure, microfibril angle (MFA), relative degree of crystallinity (%), and mechanical properties of castor fiber cell walls were investigated using X-ray diffraction (XRD) and nanoindentation. The influence of chemical composition and MFA on the mechanical properties of fiber cell wall was studied as well. The cortex of castor stalks primarily contains long fibers, while the xylem of castor stalk, an excellent wood-type material, comprises most of the castor stalk (83.95% by weight); the pith of the stalk is composed of parenchyma cells. The average elastic modulus of fiber cell wall in lower, upper, and branch parts are 16.0 GPa, 18.6 GPa, and 13.2 GPa, respectively. The average hardness of fiber cell wall in lower, upper, and branch parts are 0.50 GPa, 0.54 GPa, and 0.43 GPa, respectively. As lignin content increases from 15.57% to 17.41% and MFA decreases from 21.3˚ to 15.4˚, the elastic modulus increases from 13.2 GPa to 18.6 GPa and the hardness increases from 0.43 GPa to 0.54 GPa. The mechanical properties, including the elastic modulus and the hardness of the fiber cell wall in the upper region of the castor stalk, are higher than those in the lower region, while the mechanical properties of the fiber cell wall in the branches are lower than those in either the upper or lower regions.