The study systematically explored the effect of alkali concentration and soaking time on the microstructure and tensile properties of single-cellulosic Buluh Semantan. Scanning electron microscopy and tensile tests were conducted to determine the effects of different alkali treatments on the properties of the single-cellulosic bamboo fibers. In particular, the effects of NaOH concentration and soaking time on the tensile properties of the single-cellulosic bamboo fiber were investigated. The single-cellulosic bamboo fiber was immersed in 2, 4, 6, and 8 wt.% aqueous NaOH solutions for soaking times of 1, 3, 6, 12, 18, and 24 h. The tensile properties of the fiber increased after each alkali treatment. The alkali concentration and soaking time significantly affected the fiber properties. The ultimate tensile strength of the single-cellulosic Buluh Semantan treated with 2 wt.% NaOH for 12 h decreased to 214 MPa relative to the fibers that experienced water retting. The highest tensile strength herein was 356.8 MPa for the single-cellulosic fiber that was soaked for 12 h in 4 wt.% NaOH. Comparatively, the tensile strength of the single-cellulosic bamboo fiber that was soaked for 12 h in 8 wt.% NaOH was 234.8 MPa. The tensile modulus of the single-cellulosic fiber was 12.06 GPa after soaking in 8 wt.% NaOH for 18 h, indicating that a strong alkali treatment negatively affected the stiffness and suitability for use of the fibers in applications. The topography of the fiber surface became much rougher after the alkali treatments due to the removal of hemicellulose and other surface impurities. The alkali treatments substantially changed the morphology of the fiber surface, suggesting an increase in wettability.