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Due to its hydrophilic tendencies, the modification of cellulose nanocrystals (CNC) is needed for applying in hydrophobic drug delivery system. The CNC are chosen as a potential drug carrier because it is safety for consumption and cannot be digested by human. Previous studies have investigated several modification agents, such as hexadecyltrimethylammonium (HDTMA) and cetyl trimethylammonium bromide (CTAB), to enhance the hydrophobicity of the CNC. Natural surfactants, such as rarasaponins (RS), are suitable to avoid the human health and environmental problems caused by the use of the previous modification agents. In this work, RS were attached to the surface of CNC from bamboo shoots (BS) by hydrogen bindings. The OH peak of the CNC/RS showed the higher lever compared to the initial CNC in the FTIR analysis. The initial concentration of RS and the temperature were studied to obtain the best condition of the modification process among the variables studied. Both variables have significances toward the q as the response, where is proven by the p-value less than 5%. The highest amount of linked-RS on the CNC (q) as big as 203.81 mg/g was obtained at a RS initial concentration of 2000 ppm and a temperature of 30C.