Preparation of sludge-derived mesoporous carbon materials (SMCs) through pyrolysis of excess activated sludge from urban municipal sewage plants is an effective means of reducing pollution and utilizing a waste resource. This paper presented a method of SMC preparation in which calcium oxide (CaO), polyacrylamide (PAM), and chitosan (CAS) flocculating agents were used as pore-forming additives. Physical and chemical characterizations of the prepared SMCs were conducted by scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), Fourier transform infrared (FTIR), and X-ray photoelectron spectroscopy (XPS). The prepared SMCs were used to adsorb a tetracycline (TC) antibiotic pollutant. The influences of pH, adsorption time, temperature, and pollutant concentration on TC adsorption capacity were determined. The experiments demonstrated that weakly acidic conditions were conducive to TC adsorption, which mainly occurs via electrostatic and π-π interactions. The TC adsorption process by SMCs conformed better to the pseudo-second-order models, indicating that chemical adsorption was the dominant adsorption process. The isothermal adsorption of TC by the SMCs conformed to the Freundlich model. This implied that TC easily adhered onto the SMC surfaces via multilayer homogeneous adsorption. Thermodynamic studies revealed that the adsorption of TC onto SMCs was spontaneous and endothermic.