Inspired by wet-cool/dry-hot cycle drived prebiotic reactions, a green and efficient dry-wet cycle modification method was proposed for the preparation of polypeptide-modified bamboo fiber (P-MBF). Functionalization of P-MBF was characterized by Fourier transform infrared spectroscopy, X-ray diffraction, element analysis and scanning electron microscopy. Compared to raw bamboo fiber materials, P-MBF showed better dispersibility in aqueous solutions, and thus exhibited better adsorption performance for glycopeptide antibiotics in sewage treatment. With vancomycin as the target antibiotic, adsorption performance of P-MBF was studied in aqueous solution. Adsorption kinetics and isotherms were well correlated with pseudo-second-order model and Langmuir model, respectively. Investigation of thermodynamic parameters implied that the adsorption was a spontaneous exothermic process. The adsorption efficiencies in standard solution and drinking water were 97.83% and 91.32% , respectively. This study provides a green, efficient and economical modified bamboo fiber material for the removal of glycopeptide antibiotics from sewage samples.