In this study, used tea leaves (UTLs) were pyrolyzed to obtain used tea-leaf biochar (UTC), and then the UTC was used as an adsorbent to remove ciprofloxacin (CIP) from aqueous solutions. Batch experiments were conducted to investigate the CIP adsorption performance and mechanism. The results showed that the CIP-adsorbing ability first increased and then declined as the UTC pyrolysis temperature increased. The UTC obtained at 450°C presented excellent CIP-absorbing ability at pH 6 and 40°C. The maximum monolayer adsorption capacity was 238.10 mg/g based on the Langmuir isotherm model. The pseudo-second-order kinetic equation agreed well with the CIP adsorption process, which was controlled by both external boundary layer diffusion and intra-particle diffusion. The characterization analysis revealed that the -OH groups, C=C bonds of aromatic rings, C-H groups in aromatic rings and phenolic C-O bonds play vital roles in the CIP adsorption process, and that the N-C, N-O, O-C=O and C-OH groups of UTC were consumed in large quantities. π–π interactions, hydrogen bonding and electrostatic attraction are inferred as the main adsorption mechanisms. The present work provides not only a feasible and promising approach for UTLs utilization but also a potential adsorbent material for removing high concentrations of CIP from aqueous solutions.