In this study, spent bleaching earth (SBE) and pyrolyzed SBE (SBE@C) were tested for their capacity to remove tetracycline hydrochloride (TCH) from aqueous solution. The maximum adsorption capacity obtained by the Langmuir model is 0.114 mmol/g for SBE@C and 0.087 mmol/g for SBE. The deleterious effects of coexisting cations were ranked in a decline: Al3+ > Mg2+ > Na+. The results of adsorption various characterization methods show that the adsorption mechanisms mainly included pi-pi interactions, hydrogen bonding, electrostatic interactions, and changes in physical and chemical properties. After 3 repeated cycles of pyrolysis, the adsorption capacity of SBE@C remained at 85.4%, with SBE@C potentially recycled 21 times before complete loss of adsorption capacity. Furthermore, the problem of secondary pollution caused by SBE and residual oil is resolved by the use of SBE@C. All results indicate that SBE@C is a likely candidate for the treatment of TCH wastewater in the coming practical applications.