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This study aims to prepare bamboo-fiber-reinforced cement composites and provide a solution to the issue of poor interfacial adhesion between bamboo fibers and cement matrix. The original bamboo fibers were modified by three moderately low-cost and easy-to-handle treatments including glycerol, aluminate ester, and silane treatments. The performance of the modified bamboo-fiber-reinforced cement composites was evaluated by a series of mechanical and durability tests, including flexural and compressive strength, water absorption, chloride ion penetration, drying shrinkage, freeze–thaw resistance, and carbonization. In addition, the microstructures of composites were characterized using a scanning electron microscope (SEM). The results showed that the composites reinforced with glycerol-modified bamboo fibers had 14% increased flexural strength and comparable compressive strength. From durability perspectives, all treatments showed similar performance in drying shrinkage, whereas aluminate ester treatment was the most effective in terms of impermeability, chloride resistance, freeze–thaw resistance, and carbonization. The results could provide insights to efficient and effective natural fiber treatment to enable better performance of natural-fiber-reinforced cement-based materials. [ABSTRACT FROM AUTHOR]