This study explored the impact of sodium hydroxide and benzoylation treatment on the production of cellulose nanocrystals from Semantan bamboo (Gigantochloa scortechinii). Bamboo cellulose nanocrystals (BCNs) were obtained via acid hydrolysis, with the effectiveness of an isolation method and chemical treatments demonstrated in removing non-cellulosic constituents. X-ray diffraction analysis revealed a crystalline cellulose II structure for benzoylated BCN (B) and a crystalline cellulose I structure for NaOH-treated BCN (S), with BCN (S) exhibiting a higher crystallinity index (80.55 %) compared to BCN (B) (67.87 %). The yield of BCN (B) (23.68 ± 1.10 %) was higher than BCN (S) (20.65 ± 2.21 %). Transmission electron microscopy images showed a mean diameter of 7.95 ± 2.79 nm for BCN (S) and 9.22 ± 3.38 nm for BCN (B). Thermogravimetric analysis indicated lower thermal stability for BCN (B) compared to BCN (S), with charcoal residues at 600 °C of 31.06 % and 22 %, respectively. Zeta potential values were −41.60 ± 1.97 mV for BCN (S) and −21.80 ± 2.54 mV for BCN (B). Gigantochloa scortechinii holds significant potential for sustainable and eco-friendly applications in the construction, furniture, and renewable energy industries. These findings highlight the versatility and potential of BCNs derived from Gigantochloa scortechinii for various applications.