A large amount of spent coffee grounds is produced as a processing waste each year during making the coffee beverage. Sulfonamide antibiotics (SAs) are frequently detected in the environment and cause pollution problems. In this study, biochar (BC) and hydrochar (HC) were derived from spent coffee grounds through pyrolysis and hydrothermal carbonization, respectively. Their characteristics and sulfonamide antibiotics adsorption were investigated and compared with reference to adsorption capacity, adsorption isotherm and kinetics. Results showed BC possessed more carbonization and less oxygen-containing functional groups than HC when checked by Elemental Analysis, X-ray diffraction, X-ray photoelectron spectrometry and Fourier transform infrared. These groups affected the adsorption of sulfonamide antibiotics and adsorption mechanism. The maximum adsorption capacities of BC for sulfadiazine (SDZ) and sulfamethoxazole (SMX) were 121.5 μg/g and 130.1 μg/g at 25 °C with the initial antibiotic concentration of 500 μg/L, respectively. Meanwhile the maximum adsorption capacities of HC were 82.2 μg/g and 85.7 μg/g, respectively. Moreover, the adsorption mechanism for SAs adsorbed onto BC may be dominated by π-π electron donor-acceptor interactions, yet the SAs adsorption to HC may be attributed to hydrogen bonds. Further analysis of the adsorption isotherms and kinetics, found that physical and chemical interactions were involved in the SAs adsorption onto BC and HC. Overall, results suggested that: firstly, pyrolysis was an effective thermochemical conversion of spent coffee grounds; and secondly, BC was the more promising adsorbent for removing sulfonamide antibiotics.