The development of adsorption methods for the remediation of antibiotics pollution in water is hindered by the lack of high-performance sorbents. In this study, a nanofiber carbon aerogel was prepared using bacterial cellulose and its adsorption performances for three common antibiotics (norfloxacin, sulfamethoxazole, and chloramphenicol) in water were evaluated. The as-prepared nanofiber carbon aerogel showed a higher adsorption capacity toward target antibiotics compared to other adsorbents reported in the literature. The maximum adsorption capacities for norfloxacin, sulfamethoxazole, and chloramphenicol were 1,926, 1,264, and 525 mg/g, respectively at 298 K. Notably, the nanofiber carbon aerogel was able to adsorb 80% of the equilibrium adsorption capacity within 1 min and reach equilibrium within 15 min. After five regeneration cycles, the adsorption capacity still reached 1,166, 847, and 428 mg/g for norfloxacin, sulfamethoxazole, and chloramphenicol, respectively. The characterization results showed that the carbon aerogel exhibited a high specific surface area (1,505 m2/g) and a layered porous network structure. Furthermore, the mechanistic study reveals that the enhanced antibiotic adsorption by the as-prepared nanofiber carbon aerogel was attributed to the pore filling effect, hydrogen bonding, hydrophobic effect, electrostatic interaction, and π-π interactions. Overall, these results imply that low-cost and green nanofiber carbon aerogels may be promising adsorbents for the remediation of antibiotic-contaminated wastewater. The materials prepared from natural and readily available bacterial cellulose can adsorb antibiotics efficiently, which provides a reference for the development of adsorbent materials using natural substances.