A limited number of studies have been conducted on the relationship between serum vitamin levels and pulmonary function, particularly in the elderly population. This study attempted to confirm the association between serum vitamin levels (folate, vitamin A, and vitamin E) and pulmonary function in the elderly population of Korea. A total of 1166 subjects (528 men and 637 women) participated in the Korean National Health and Nutrition Examination Survey from 2016 to 2018. Serum levels of folate, vitamin A, and vitamin E were measured in the subjects. The subjects’ pulmonary function measurement items were as follows: forced vital capacity (FVC), forced expiratory volume in one second (FEV1), forced expiratory volume in one second/forced vital capacity (FEV1/FVC), forced expiratory flow at 25% and 75% of the pulmonary volume (FEF25–75%), forced expiratory volume in 6 s (FEV6), and peak expiratory velocity (PEV). We performed regression analysis considering FEV1, PEV, FVC, FEF25–75%, and FEV1/FVC and FEV6 as dependent variables. Serum vitamin A levels were not associated with pulmonary function. In elderly men, serum vitamin E levels were negatively correlated with FVC [B = − 0.012, 95% confidence interval (CI) − 0.022 to − 0.003, p = 0.012] and FEV1 (B = − 0.010, 95% CI − 0.115 to − 0.007, p = 0.028). We confirmed a positive correlation of the serum folate level with FEV1 (B = 0.017, 95% CI 0.004–0.030, p = 0.009), FEV1/FVC (B = 0.003, 95% CI 0.001–0.005, p = 0.007), and FEF25–75% (B = 0.031, 95% CI 0.010–0.053, p = 0.005) in elderly men. This study confirmed that high serum folate levels were positively associated with pulmonary function in elderly men in Korea. Further studies are needed to understand the longitudinal effect of folate and its biological mechanism in pulmonary function.