RS1 is a high aluminum resistant Rhodotorula taiwanensis strain selected from acid soil of oil tea in Yingtan of Jiangxi Province, which can tolerate aluminum concentration up to 200 mmol/L. Previous studies have showed that RS1 can immobilize aluminum on the cell surface and block it from entering the cell. However, it is unclear what kind of group on the cell surface is involved in aluminum fixation. In this paper, Fourier transform infrared spectroscopy and Raman spectroscopy were used to study the surface functional group changes of RS1 cells under aluminum stress in order to explore the high aluminum resistance mechanism of RS1 from the perspective of spectroscopy. It was found that the absorption peak at 1 403 cm^-1 in the IR spectrum of RS1 was red shifted to 1 397 cm^-1 after treatment with 70 mmol/L aluminum for 24 h, which may be a carboxyl group. A new absorption peak appeared at 1 706 cm^-1, which may be a carbonyl peak. The absorption peak intensities of amide I band in the IR spectrum with aluminum treatment were significantly increased and the mannan peak disappeared. The new absorption peaks of the Raman spectrum at 779 cm^-1, 856 cm^-1 and 1 270 cm^-1 may be the absorption peaks of RNA, tyrosine and amide Ш band, respectively. The results of IR and Raman spectroscopy show that the substances related to aluminum adsorption on the surface of RS1 cells are mainly polysaccharides and proteins of cell wall, and the main functional groups include carboxyl groups, carbonyl groups and amide groups. The immobilization of aluminum by these functional groups on cell surface may be an important mechanism for the high aluminum tolerance of Rhodotorula taiwanensis RS1.